JP2012212506A - Laminate type battery - Google Patents

Laminate type battery Download PDF

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JP2012212506A
JP2012212506A JP2009156735A JP2009156735A JP2012212506A JP 2012212506 A JP2012212506 A JP 2012212506A JP 2009156735 A JP2009156735 A JP 2009156735A JP 2009156735 A JP2009156735 A JP 2009156735A JP 2012212506 A JP2012212506 A JP 2012212506A
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positive electrode
negative electrode
external terminal
sheet
laminated
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Tetsuo Kawai
徹夫 川合
Yasuo Arishima
康夫 有島
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Maxell Holdings Ltd
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Hitachi Maxell Ltd
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Priority to JP2009156735A priority Critical patent/JP2012212506A/en
Priority to PCT/JP2010/061266 priority patent/WO2011002064A1/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
    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/543—Terminals
    • H01M50/547—Terminals characterised by the disposition of the terminals on the cells
    • H01M50/548—Terminals characterised by the disposition of the terminals on the cells on opposite sides of the cell
    • 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
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/531—Electrode connections inside a battery casing
    • H01M50/54—Connection of several leads or tabs of plate-like electrode stacks, e.g. electrode pole straps or bridges
    • 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
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/543—Terminals
    • H01M50/547—Terminals characterised by the disposition of the terminals on the cells
    • H01M50/55—Terminals characterised by the disposition of the terminals on the cells on the same side of the cell
    • 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
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/543—Terminals
    • H01M50/552—Terminals characterised by their shape
    • H01M50/553—Terminals adapted for prismatic, pouch or rectangular cells
    • H01M50/557—Plate-shaped terminals
    • 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
    • H01M50/50—Current conducting connections for cells or batteries
    • H01M50/543—Terminals
    • H01M50/564—Terminals characterised by their manufacturing process
    • H01M50/566—Terminals characterised by their manufacturing process by welding, soldering or brazing
    • 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

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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)
  • Sealing Battery Cases Or Jackets (AREA)
  • Connection Of Batteries Or Terminals (AREA)

Abstract

PROBLEM TO BE SOLVED: To provide a laminate type battery which incorporates a laminated electrode body which is laminated in many layers or a wound electrode body which is wound a number of times and, therefore, exhibits high reliability and also gives high degree of freedom to an external terminal pull-out position.SOLUTION: The laminate type battery, or a battery whose electrode body having a sheet-like cathode, a sheet-like anode and a separator is accommodated in a laminate film outer package, includes a laminated electrode body whose electrode consists of 20 or more laminated layers or a wound electrode body which is wound 10 times or more, and is constructed in such a way that a cathode tab laminate consisting of plural laminated cathode tabs concerned with the sheet-like cathode is divided into plural portions, which respectively are connected to separate external cathode terminals, each of the external cathode terminals being electrically connected together to one another inside or outside the laminate film outer package, and that an anode tab laminate consisting of plural laminated anode tabs concerned with the sheet-like anode is divided into plural portions, which respectively are connected to separate external cathode terminals, each of the external anode terminals being electrically connected together to one another inside or outside the laminate film outer package.

Description

本発明は、積層数の多い積層電極体や巻回数の多い巻回電極体を備えており、高い信頼性を有するラミネート形電池に関するものである。   The present invention relates to a laminated battery having a high reliability with a laminated electrode body having a large number of laminated layers and a wound electrode body having a large number of turns.

近年では、電池の用途が拡大するにつれて、高容量化や、高エネルギー密度化、高出力化といった電池の特性向上を目的とした開発が盛んに行われている。特に、自動車用途などの高出力、高容量が要求される用途への電池の適用も求められるようになっており、従来はニッケル水素電池が用いられてきたが、最近では、より軽量化を図り得るリチウムイオン二次電池の適用も検討されている。   In recent years, as the use of batteries has expanded, development aimed at improving battery characteristics such as higher capacity, higher energy density, and higher output has been actively conducted. In particular, the application of batteries to applications that require high output and high capacity, such as automobile applications, has been required, and nickel-metal hydride batteries have been used in the past. Application of the obtained lithium ion secondary battery is also being studied.

ところで、電池の高容量化を図るには、電池内に導入する活物質量を増やすことが有効であり、また、電池の負荷特性向上を図るには、電極を薄くし、反応面積を増やすことが有効である。   By the way, it is effective to increase the amount of active material introduced into the battery in order to increase the capacity of the battery, and to improve the load characteristics of the battery, the electrode is made thinner and the reaction area is increased. Is effective.

例えば一般的な円筒形の１８６５０型電池を前記のような高容量、高出力が要求される用途に使用するには、数百個から数千個を用いる必要があり、それらの電池をシリーズやパラレルに組電池とすることも不可能ではないが、作業が非常に煩雑となり、信頼性の確保も困難となる。   For example, in order to use a general cylindrical 18650 type battery for an application requiring high capacity and high output as described above, it is necessary to use hundreds to thousands of batteries. Although it is not impossible to form an assembled battery in parallel, the work becomes very complicated and it is difficult to ensure reliability.

そこで、こうした問題を解決するには、１個の電池を大型化し、例えば組電池に用いる単電池の使用個数を減らすことが有効である。そして、現在では、１個で１０Ａｈを超えるような大型の電池の開発も進みつつある。   In order to solve these problems, it is effective to increase the size of one battery and reduce the number of single cells used for, for example, an assembled battery. At present, development of a large battery exceeding 10 Ah by one piece is also in progress.

前記のような大型電池としては、例えば、集電体の表面に正極合剤層を有する正極と集電体の表面に負極合剤層を有する負極とをセパレータを介して積層した積層電極体を用いる電池の場合には、正極および負極の積層数を多くしたものが挙げられ（例えば、特許文献１）、また、集電体の表面に正極合剤層を有する正極と集電体の表面に負極合剤層を有する負極とをセパレータを介して重ね、渦巻き状に巻回した巻回電極体を用いる電池の場合には、巻回数を多くしたものが挙げられる。   As such a large battery, for example, a laminated electrode body in which a positive electrode having a positive electrode mixture layer on the surface of a current collector and a negative electrode having a negative electrode mixture layer on the surface of the current collector are laminated via a separator. In the case of a battery to be used, one having a larger number of positive and negative electrode layers (for example, Patent Document 1) is used, and the positive electrode and the current collector surface having a positive electrode mixture layer on the current collector surface. In the case of a battery using a spirally wound electrode body that is wound with a negative electrode having a negative electrode mixture layer via a separator and wound in a spiral shape, a battery having a larger number of windings may be mentioned.

また、前記のような大型電池では、形状自由度が高く軽量であるといった利点から、金属ラミネートフィルムで構成されるラミネートフィルム外装体が使用される場合が多い。そして、前記のような電池の電極からの集電は、集電体の一部を正極合剤層や負極合剤層を形成せずに無地部とし、かかる箇所を集電タブとして外部端子と溶接（超音波溶接など）などによって接続して行うことが一般的である。   Moreover, in the large battery as described above, a laminate film outer package composed of a metal laminate film is often used because of its advantage of high shape flexibility and light weight. And the current collection from the electrode of the battery as described above is to make a part of the current collector a plain part without forming a positive electrode mixture layer or a negative electrode mixture layer, and such a point as a current collecting tab and an external terminal. In general, the connection is performed by welding (ultrasonic welding or the like).

特許第３６８３２４２号公報Japanese Patent No. 3683242

しかしながら、前記のように電極の積層数の多い積層電極体を有する電池や、巻回数の多い巻回電極体を有する電池では、電極体の厚みが大きくなる。よって、外部端子と距離のある電極に係る集電タブは、外部端子との接続のために長い距離を引き回す必要があり、その際に集電タブに大きな張力がかかることになって破損が生じる虞がある。このようなことから、通常は、集電タブを電極端面に沿わせて引き回すなどして集電タブにかかる張力を低減する方策が取られているが、この場合、集電タブが非常に長くなるため、抵抗が増大してしまう。   However, in a battery having a laminated electrode body with a large number of laminated electrodes as described above or a battery having a wound electrode body with a large number of turns, the thickness of the electrode body becomes large. Therefore, the current collecting tab related to the electrode having a distance from the external terminal needs to be routed over a long distance for connection to the external terminal, and in this case, a large tension is applied to the current collecting tab, resulting in damage. There is a fear. For this reason, usually, measures are taken to reduce the tension applied to the current collecting tab by, for example, drawing the current collecting tab along the electrode end face. In this case, however, the current collecting tab is very long. Therefore, the resistance increases.

また、電極の積層数を増やした積層電極体を有する電池や、巻回数を増やした巻回電極体を有する電池では、多数の集電タブを積層して外部端子に溶接することから、集電タブと外部端子との溶接箇所の信頼性も低下する。   In addition, in a battery having a laminated electrode body with an increased number of electrode layers and a battery having a wound electrode body with an increased number of turns, a large number of current collecting tabs are stacked and welded to an external terminal. The reliability of the welded portion between the tab and the external terminal is also lowered.

例えば、電極の集電タブの一部を外部端子の片面に溶接し、残りを外部端子の他面に溶接する手法や、外部端子の幅を大きくして、電極の集電タブの一部を重ねて外部端子の所定箇所に溶接し、集電タブの残りを重ねて外部端子の別の箇所に溶接する手法によって、前記のような問題を回避することも考えられる。しかし、前者の手法では、多数の集電タブを一度に溶接することに変わりはなく、集電タブと外部端子との溶接信頼性が不十分となる虞がある。また、後者の手法では、集電タブと外部端子との溶接が複数回に分けて行われることから、後の溶接時に先に溶接した箇所に振動などが加わるなどして悪影響を及ぼす虞があり、外部端子の幅や長さが大きくなることで、電池内空間の利用の点で不利となり、外部端子を外装体から引き出す位置の自由度が損なわれる問題もある。   For example, a method of welding a part of the electrode current collector tab to one side of the external terminal and welding the rest to the other surface of the external terminal, or increasing the width of the external terminal, It is also conceivable to avoid the above-described problem by a method of overlapping and welding to a predetermined portion of the external terminal and overlapping the remaining current collecting tab and welding to another portion of the external terminal. However, in the former method, there is no change in welding a large number of current collecting tabs at once, and there is a possibility that the welding reliability between the current collecting tabs and the external terminals may be insufficient. In the latter method, since the current collector tab and the external terminal are welded in multiple steps, there is a risk of adverse effects such as vibration applied to the previously welded part during subsequent welding. In addition, the increase in the width and length of the external terminal is disadvantageous in terms of utilization of the space in the battery, and there is also a problem that the degree of freedom in the position of pulling out the external terminal from the exterior body is impaired.

本発明は前記事情に鑑みてなされたものであり、その目的は、積層数の多い積層電極体や巻回数の多い巻回電極体を備えており、信頼性が高く、また、外部端子の引き出し位置の自由度が高いラミネート形電池を提供することにある。   The present invention has been made in view of the above circumstances, and an object of the present invention is to provide a laminated electrode body having a large number of laminated layers and a wound electrode body having a large number of turns, and is highly reliable, and is capable of leading out an external terminal. An object of the present invention is to provide a laminated battery having a high degree of freedom in position.

前記目的を達成し得た本発明のラミネート形電池は、集電体の少なくとも片面に正極合剤層を有する複数のシート状正極と集電体の少なくとも片面に負極合剤層を有する複数のシート状負極とがセパレータを介して積層された積層電極体が、平面視で多角形のラミネートフィルム外装体に収容されており、前記ラミネートフィルム外装体の外周辺が熱シールされているラミネート形電池であって、前記積層電極体の有するシート状正極とシート状負極との合計数が２０以上であり、各シート状正極の集電体の一部は、正極合剤層が形成されずに正極タブとされ、各シート状負極の集電体の一部は、負極合剤層が形成されずに負極タブとされ、前記複数のシート状正極の正極タブが、複数の組に分けられて積層されることにより、複数の正極タブ積層体が形成されており、前記複数のシート状負極の負極タブが、複数の組に分けられて積層されることにより、複数の負極タブ積層体が形成されており、各正極タブ積層体は、それぞれ別の正極外部端子に接続され、かつ各負極タブ積層体は、それぞれ別の負極外部端子に接続されており、各正極外部端子および各負極外部端子は、それぞれラミネートフィルム外装体の内部および外部の少なくとも一方で互いに電気的に接続されていることを特徴とするものである。   The laminated battery of the present invention that can achieve the above object is a plurality of sheet-like positive electrodes having a positive electrode mixture layer on at least one side of a current collector and a plurality of sheets having a negative electrode mixture layer on at least one side of the current collector. A laminated battery in which a laminated electrode body in which a negative electrode is laminated via a separator is accommodated in a polygonal laminated film exterior body in a plan view, and the outer periphery of the laminated film exterior body is heat-sealed. The total number of the sheet-like positive electrode and the sheet-like negative electrode included in the laminated electrode body is 20 or more, and a part of the collector of each sheet-like positive electrode is a positive electrode tab without forming a positive electrode mixture layer. A part of the current collector of each sheet-like negative electrode is a negative electrode tab without forming a negative electrode mixture layer, and the positive electrode tabs of the plurality of sheet-like positive electrodes are divided into a plurality of sets and stacked. Multiple positive poles A laminate is formed, and a plurality of negative electrode tab laminates are formed by laminating the negative electrode tabs of the plurality of sheet-like negative electrodes into a plurality of sets, and each positive electrode tab laminate is Each negative electrode tab laminate is connected to another negative electrode external terminal, and each positive electrode external terminal and each negative electrode external terminal are respectively connected to the inside of the laminate film outer package and It is characterized in that at least one of the outsides is electrically connected to each other.

また、本発明のラミネート形電池の別の態様は、集電体の少なくとも片面に正極合剤層を有するシート状正極と集電体の少なくとも片面に負極合剤層を有するシート状負極とがセパレータを介して積層されて渦巻き状に巻回された、横断面が略長円形（長円形を含む。以下、同じ。）巻回電極体が、平面視で四角形のラミネートフィルム外装体に収容されており、前記ラミネートフィルム外装体の外周辺が熱シールされているラミネート形電池であって、前記巻回電極体の巻回数が１０以上であり、前記シート状正極の集電体の幅方向の端部は、正極合剤層が形成されずに正極タブとされ、前記シート状負極の集電体の、前記正極タブとは反対側の幅方向の端部は、負極合剤層が形成されずに負極タブとされ、前記シート状正極の正極タブは、前記巻回電極体の略長円形の平坦部において、複数の組に分けられて積層されることにより、複数の正極タブ積層体が形成されており、前記シート状負極の負極タブは、前記巻回電極体の略長円形の平坦部において、複数の組に分けられて積層されることにより、複数の負極タブ積層体が形成されており、前記正極タブ積層体は、それぞれ別の正極外部端子に接続され、かつ前記負極タブ積層体は、それぞれ別の負極外部端子に接続されており、各正極外部端子および各負極外部端子同士は、それぞれラミネートフィルム外装体の内部および外部の少なくとも一方で互いに電気的に接続されていることを特徴とするものである。   In another aspect of the laminated battery of the present invention, a sheet-like positive electrode having a positive electrode mixture layer on at least one side of a current collector and a sheet-like negative electrode having a negative electrode mixture layer on at least one side of the current collector are separators. A spirally wound electrode body that is laminated in a spiral shape and is wound in a spiral shape is accommodated in a rectangular laminate film outer package in a plan view. A laminate type battery in which an outer periphery of the laminate film exterior body is heat-sealed, wherein the number of windings of the wound electrode body is 10 or more, and an end in a width direction of the current collector of the sheet-like positive electrode The portion is formed as a positive electrode tab without forming a positive electrode mixture layer, and the negative electrode mixture layer is not formed at the end of the sheet-like negative electrode collector in the width direction opposite to the positive electrode tab. And the positive electrode tab of the sheet-like positive electrode is In the substantially oval flat portion of the wound electrode body, a plurality of positive electrode tab laminates are formed by being divided into a plurality of sets, and the negative electrode tab of the sheet-like negative electrode is In the substantially oval flat portion of the rotating electrode body, a plurality of negative electrode tab laminates are formed by being divided into a plurality of groups, and each of the positive electrode tab laminates has a different positive electrode external terminal. And the negative electrode tab laminates are respectively connected to different negative electrode external terminals, and the respective positive electrode external terminals and the respective negative electrode external terminals are at least one of the inside and the outside of the laminate film outer package, respectively. It is characterized by being electrically connected.

本発明によれば、積層数の多い積層電極体や巻回数の多い巻回電極体を備えており、信頼性が高く、また、外部端子の引き出し位置の自由度が高いラミネート形電池を提供することができる。   According to the present invention, there is provided a laminated battery having a laminated electrode body having a large number of laminated layers and a wound electrode body having a large number of turns, and having high reliability and a high degree of freedom in a position where an external terminal is drawn. be able to.

本発明のラミネート形電池の一例を模式的に示す平面図である。It is a top view which shows typically an example of the laminated battery of this invention. 本発明のラミネート形電池の他の例を模式的に示す平面図である。It is a top view which shows typically the other example of the laminated battery of this invention. 図１および図２のＡ−Ａ線における要部断面図の一例である。It is an example of principal part sectional drawing in the AA line of FIG. 1 and FIG. 図１および図２のＡ−Ａ線における要部断面図の一例である。It is an example of principal part sectional drawing in the AA line of FIG. 1 and FIG.

図１は、本発明のラミネート形電池の一例を模式的に示す平面図である。図１に示すラミネート形電池１では、電極体および電解液が、平面視で矩形のラミネートフィルム外装体２内に収容されている。そして、正極外部端子３および負極外部端子４が、ラミネートフィルム外装体２の同じ辺から引き出されている。ラミネートフィルム外装体２は、電池内側となる面に熱融着樹脂層を有する金属ラミネートフィルムにより構成されている。より具体的には、例えば２枚の金属ラミネートフィルムが重ねられてラミネートフィルム外装体２を構成し、電極体や電解液を内部に収容した状態でラミネートフィルム外装体２の外周辺が熱シールされることで、その内部が密閉されている。   FIG. 1 is a plan view schematically showing an example of a laminated battery of the present invention. In the laminated battery 1 shown in FIG. 1, the electrode body and the electrolytic solution are accommodated in a rectangular laminated film outer package 2 in a plan view. The positive external terminal 3 and the negative external terminal 4 are drawn from the same side of the laminate film outer package 2. Laminate film outer package 2 is formed of a metal laminate film having a heat-sealing resin layer on the inner surface of the battery. More specifically, for example, two metal laminate films are stacked to form a laminate film exterior body 2, and the outer periphery of the laminate film exterior body 2 is heat-sealed in a state where the electrode body and the electrolytic solution are housed inside. As a result, the inside is sealed.

また、図２は、本発明のラミネート形電池の他の例を模式的に示す平面図である。図２に示すラミネート形電池１は、正極外部端子３および負極外部端子４が、それぞれラミネートフィルム外装体２の互いに対向する辺から外部に引き出されている他は、図１に示すラミネート形電池と同様の構成である。   FIG. 2 is a plan view schematically showing another example of the laminated battery of the present invention. The laminate type battery 1 shown in FIG. 2 is the same as the laminate type battery shown in FIG. 1 except that the positive electrode external terminal 3 and the negative electrode external terminal 4 are drawn out from the opposite sides of the laminate film outer package 2. It is the same composition.

図３に、図１および図２のＡ−Ａ線における要部断面図の一例を示す。図３は、複数のシート状正極５と複数のシート状負極６とがセパレータ７を介して積層された積層電極体を有するラミネート形電池の例である。なお、図３では、図面が複雑になることを避けるため、ラミネートフィルム外装体を構成する金属ラミネートフィルムの各層を区別しておらず、また、シート状正極の正極合剤層と集電体、およびシート状負極の負極合剤層と集電体も区別していない（後記の図４も同様である。）。   FIG. 3 shows an example of a cross-sectional view of the main part taken along line AA in FIGS. 1 and 2. FIG. 3 is an example of a laminated battery having a laminated electrode body in which a plurality of sheet-like positive electrodes 5 and a plurality of sheet-like negative electrodes 6 are laminated via separators 7. In FIG. 3, in order to avoid complication of the drawing, the layers of the metal laminate film constituting the laminate film exterior body are not distinguished, and the positive electrode mixture layer and the current collector of the sheet-like positive electrode, and There is no distinction between the negative electrode mixture layer and the current collector of the sheet-like negative electrode (the same applies to FIG. 4 described later).

図３に示すラミネート形電池１において、複数のシート状正極５は、集電体の片面または両面に正極合剤層が形成されており、かつ集電体の一部（図３中右端側）に正極合剤層が形成されずに正極タブとなり、各シート状正極５の正極タブが積層されて正極タブ積層体５ａ、５ｂを構成している。そして、正極タブ積層体５ａが正極外部端子３ａに、正極タブ積層体５ｂが正極外部端子３ｂに、それぞれ接続されている。また、図示していないが、ラミネート形電池１では、複数のシート状負極６は、集電体の片面または両面に負極合剤層が形成されており、かつ集電体の一部に負極合剤層が形成されずに負極タブとなり、各シート状負極６の負極タブが積層されて、複数の負極タブ積層体が構成されている。そして、各負極タブ積層体は、それぞれ別の負極外部端子に接続されている。   In the laminated battery 1 shown in FIG. 3, the plurality of sheet-like positive electrodes 5 have a positive electrode mixture layer formed on one side or both sides of the current collector, and a part of the current collector (right end side in FIG. 3). Thus, a positive electrode tab is formed without forming a positive electrode mixture layer, and the positive electrode tabs of the respective sheet-like positive electrodes 5 are laminated to form positive electrode tab laminates 5a and 5b. The positive electrode tab laminate 5a is connected to the positive electrode external terminal 3a, and the positive electrode tab laminate 5b is connected to the positive electrode external terminal 3b. Although not shown, in the laminated battery 1, the plurality of sheet-like negative electrodes 6 have a negative electrode mixture layer formed on one side or both sides of the current collector, and a negative electrode mixture on a part of the current collector. A negative electrode tab is formed without forming the agent layer, and the negative electrode tabs of the respective sheet-like negative electrodes 6 are laminated to form a plurality of negative electrode tab laminates. Each negative electrode tab laminate is connected to a different negative external terminal.

本発明のラミネート形電池では、積層電極体を有する態様においては、かかる積層電極体におけるシート状正極とシート状負極との合計数が２０以上であるが、このように積層数の多い積層電極体を有するラミネート形電池の場合、前記の通り、外部端子との接続時（溶接時）に正負極の集電タブの破損や、集電タブと外部端子との溶接による接続が不十分となることによる信頼性低下が起こり得る。   In the laminated battery of the present invention, in the embodiment having the laminated electrode body, the total number of the sheet-like positive electrode and the sheet-like negative electrode in the laminated electrode body is 20 or more. In the case of a laminated battery having a battery, as described above, when the external terminal is connected (welding), the positive and negative current collecting tabs are damaged, and the connection between the current collecting tab and the external terminals is insufficient. Reliability degradation can occur.

そこで、本発明のラミネート形電池では、図３に示すように、複数のシート状正極の正極タブを積層した正極タブ積層体を複数に分け、各正極タブ積層体をそれぞれ別の正極外部端子に接続し、各正極外部端子を重ねるなどすることにより、各正極外部端子をラミネートフィルム外装体の内部および外部の少なくとも一方で互いに電気的に接続しつつラミネートフィルム外装体の外部に引き出している。また、図示していないが、本発明のラミネート形電池では、複数のシート状負極についても、それらの負極タブを積層した負極タブ積層体を複数に分け、各負極タブ積層体をそれぞれ別の負極外部端子に接続し、各負極外部端子を重ねるなどすることにより、各負極外部端子をラミネートフィルム外装体の内部および外部の少なくとも一方で互いに電気的に接続しつつラミネートフィルム外装体の外部に引き出している。   Therefore, in the laminated battery of the present invention, as shown in FIG. 3, a positive electrode tab laminate in which a plurality of sheet-like positive electrode tabs are laminated is divided into a plurality of pieces, and each positive electrode tab laminate is provided as a separate positive electrode external terminal. The positive electrode external terminals are pulled out to the outside of the laminate film exterior body while being electrically connected to each other at least one of the inside and the outside of the laminate film exterior body by connecting and overlapping each positive electrode external terminal. Although not shown, in the laminated battery of the present invention, the negative electrode tab laminate in which the negative electrode tabs are laminated is divided into a plurality of sheet-like negative electrodes, and each negative electrode tab laminate is divided into a separate negative electrode. By connecting to the external terminal and overlapping each negative electrode external terminal, each negative electrode external terminal is pulled out to the outside of the laminate film exterior body while being electrically connected to at least one of the inside and outside of the laminate film exterior body. Yes.

そのため、本発明のラミネート形電池では、積層電極体に係る電極数を多くしつつ、１つの正極タブ積層体や１つの負極タブ積層体では、正極タブ、負極タブの積層数を減らし、かつ、１つの正極外部端子や１つの負極外部端子に接続する正極タブ数、負極タブ数を減らすことができる。よって、正極タブ積層体と正極外部端子との溶接強度、および負極タブ積層体と負極外部端子との溶接強度を高めて、これらの間の電気的接続を良好にすることができる。また、正極外部端子や負極外部端子を複数にすることで、シート状正極と正極外部端子との距離およびシート状負極と負極外部端子との距離を可及的に短くして、正極タブや負極タブの距離が長くなることによる電池製造時の破損や、抵抗の増大を抑制することができる。本発明のラミネート形電池では、これらの作用によって、高い信頼性を確保することができる。   Therefore, in the laminated battery of the present invention, while increasing the number of electrodes related to the laminated electrode body, in one positive electrode tab laminated body or one negative electrode tab laminated body, the number of laminated positive electrode tabs and negative electrode tabs is reduced, and The number of positive electrode tabs and the number of negative electrode tabs connected to one positive electrode external terminal or one negative electrode external terminal can be reduced. Therefore, the welding strength between the positive electrode tab laminate and the positive electrode external terminal and the welding strength between the negative electrode tab laminate and the negative electrode external terminal can be increased, and the electrical connection therebetween can be improved. Moreover, by using a plurality of positive electrode external terminals and negative electrode external terminals, the distance between the sheet-like positive electrode and the positive electrode external terminal and the distance between the sheet-like negative electrode and the negative electrode external terminal are made as short as possible, and the positive electrode tab and the negative electrode It is possible to suppress damage during battery manufacturing and increase in resistance due to the long tab distance. In the laminated battery of the present invention, high reliability can be secured by these actions.

しかも、本発明のラミネート形電池では、正極外部端子および負極外部端子を複数枚使用し、それぞれをラミネートフィルム外装体の内部および外部の少なくとも一方で互いに電気的に接続されているため、各正極外部端子の電気的接続方法および各負極外部端子の電気的接続方法の選択によって、ラミネートフィルム外装体から外部端子を引き出す位置を容易に変更し得ることから、外部端子の引き出し位置の自由度が高く、本発明のラミネート形電池の使用機器の設計上の自由度も高くなる。   Moreover, in the laminated battery of the present invention, a plurality of positive electrode external terminals and negative electrode external terminals are used, and each of them is electrically connected to at least one of the inside and the outside of the laminate film exterior body. By selecting the electrical connection method of the terminal and the electrical connection method of each negative electrode external terminal, the position where the external terminal is drawn out from the laminate film exterior body can be easily changed, so the degree of freedom of the external terminal drawing position is high, The degree of freedom in designing the device using the laminated battery of the present invention is also increased.

ラミネート形電池に係る各正極外部端子の電気的接続方法および各負極外部端子の電気的接続方法の好適例としては、例えば、図３に示すように、各正極外部端子同士および各負極外部端子同士を、それぞれラミネートフィルム外装体の内部で重ねる方法が挙げられる。各正極外部端子同士をラミネートフィルム外装体の内部で重ね、かつ各負極外部端子同士をラミネートフィルム外装体の内部で重ねた上で、これらをラミネートフィルム外装体から引き出すことで、例えば、平面視での面積を大きくすることなく（例えば、正極外部端子や負極外部端子の図１に示す横方向の長さを長くすることなく）、正極外部端子の総断面積や負極外部端子の総断面積を大きくできる。   As a suitable example of the electrical connection method of each positive electrode external terminal and the electrical connection method of each negative electrode external terminal related to the laminate type battery, for example, as shown in FIG. Can be included in the laminate film outer package. Each positive external terminal is overlapped inside the laminate film exterior body, and each negative electrode external terminal is overlapped inside the laminate film exterior body, and these are pulled out from the laminate film exterior body, for example, in plan view Without increasing the area (for example, without increasing the lateral length of the positive electrode external terminal and the negative electrode external terminal shown in FIG. 1), the total cross sectional area of the positive external terminal and the total cross sectional area of the negative external terminal Can be big.

例えば、大電流放電が要求される電池では、正極外部端子や負極外部端子の断面積を大きくする必要があり、通常は平面視での幅を広げることで対応している。ところが、正極外部端子や負極外部端子の幅を広げると、正極外部端子と負極外部端子との接触による短絡が発生しやすくなる問題から、例えば、図１に示すようにラミネートフィルム外装体の同一辺から正極外部端子と負極外部端子とを引き出すことが難しくなり、外部端子の引き出し位置の自由度が損なわれてしまう。他方、１枚の正極外部端子や１枚の負極外部端子を厚くすることで断面積を大きくした場合、多数の電極に係る集電タブを積層したタブ積層体と、厚みの大きな外部端子とを溶接することになるため、溶接箇所の信頼性が低下する。   For example, in a battery that requires a large current discharge, it is necessary to increase the cross-sectional area of the positive external terminal and the negative external terminal, and this is usually dealt with by increasing the width in plan view. However, when the width of the positive electrode external terminal or the negative electrode external terminal is increased, a short circuit due to contact between the positive electrode external terminal and the negative electrode external terminal is likely to occur. For example, as shown in FIG. Thus, it is difficult to pull out the positive electrode external terminal and the negative electrode external terminal from the position, and the degree of freedom of the position where the external terminal is pulled out is impaired. On the other hand, when the cross-sectional area is increased by thickening one positive external terminal or one negative external terminal, a tab laminate in which current collecting tabs related to a large number of electrodes are stacked, and a thick external terminal Since it will weld, the reliability of a welding location falls.

しかしながら、本発明のラミネート形電池では、前記の通り、各正極外部端子同士の電気的接続方法および各負極外部端子同士の電気的接続方法の選択によって、例えば正極外部端子や負極外部端子の平面視での幅を広げることなしに、正極外部端子の総断面積や負極外部端子の総断面積を大きくでき、しかも、前記の通り、１枚の正極外部端子や１枚の負極外部端子に溶接される正極タブ積層体や負極タブ積層体の積層数を少なくできるため、溶接箇所の信頼性も高め得る。よって、本発明のラミネート形電池は、大電流放電が可能であり、かつ高い信頼性が損なわれることなく、ラミネートフィルム外装体から外部端子を引き出す位置の自由度が高くなる。   However, in the laminated battery of the present invention, as described above, for example, in a plan view of the positive external terminal and the negative external terminal, depending on the selection of the electrical connection method between the positive external terminals and the electrical connection method between the negative external terminals. Without increasing the width, the total cross-sectional area of the positive external terminal and the total cross-sectional area of the negative external terminal can be increased, and as described above, it is welded to one positive external terminal or one negative external terminal. Since the number of stacked positive electrode tab laminates and negative electrode tab laminates can be reduced, the reliability of the welded portion can be improved. Therefore, the laminated battery of the present invention can discharge a large current and has a high degree of freedom in the position where the external terminal is drawn from the laminated film outer package without impairing high reliability.

なお、積層電極体を有する本発明のラミネート形電池において、正極タブ積層体および負極タブ積層体の数は、複数であればよく、少なくとも２以上であるが、通常は５以下であり、４以下であることが好ましく、３以下であることがより好ましい。また、１つの正極タブ積層体における正極タブの積層数は、５〜６０であることが好ましく、１つの負極タブ積層体における負極タブの積層数は、５〜６０であることが好ましい。   In the laminated battery of the present invention having a laminated electrode body, the number of positive electrode tab laminates and negative electrode tab laminates may be plural and is at least 2 but usually 5 or less and 4 or less. It is preferable that it is 3 or less. Moreover, it is preferable that the lamination | stacking number of the positive electrode tab in one positive electrode tab laminated body is 5-60, and it is preferable that the lamination | stacking number of the negative electrode tab in one negative electrode tab laminated body is 5-60.

図４に、図１および図２のＡ−Ａ線における要部断面図の他の例を示す。図４は、複数のシート状正極５と複数のシート状負極６とがセパレータ７を介して積層され、更に渦巻き状に巻回された巻回電極体（横断面が略長円形の巻回電極体）を有するラミネート形電池の例である。なお、図４では、各構成要素の理解を容易にするために、ラミネートフィルム外装体２と巻回電極体の最外周部（正極集電体５１）との間、および巻回電極体の巻回中心部（負極集電体６１、６１）に隙間を入れている。   FIG. 4 shows another example of a cross-sectional view of the main part taken along line AA in FIGS. FIG. 4 shows a wound electrode body in which a plurality of sheet-like positive electrodes 5 and a plurality of sheet-like negative electrodes 6 are laminated via separators 7 and wound in a spiral shape (a wound electrode having a substantially elliptical cross section). This is an example of a laminated battery having a body. In FIG. 4, in order to facilitate understanding of each component, between the laminate film outer package 2 and the outermost peripheral portion (positive electrode current collector 51) of the wound electrode body, and the winding of the wound electrode body. A gap is formed in the center of rotation (the negative electrode current collectors 61 and 61).

図４に示すラミネート形電池１において、シート状正極５は、集電体の片面または両面に正極合剤層が形成されており、かつ集電体の幅方向の端部（図４中右端側）に正極合剤層が形成されずに正極タブとなり、この正極タブが、巻回電極体の略長円形の平坦部において複数の組に分けられて正極タブ積層体５ａ、５ｂを形成している。そして、正極タブ積層体５ａが正極外部端子３ａに、正極タブ積層体５ｂが正極外部端子３ｂに、それぞれ接続されている。また、図示していないが、ラミネート形電池１では、シート状負極６は、集電体の片面または両面に負極合剤層が形成されており、かつ集電体の、正極タブとは反対側の端部（図中左側の端部）に負極合剤層が形成されずに負極タブとなり、この負極タブが、巻回電極体の略長円形の平坦部において複数の組に分けられて複数の負極タブ積層体が形成されている。そして、各負極タブ積層体は、それぞれ別の負極外部端子に接続されている。なお、図４に示す電池に係る巻回電極体において、最外周部は、シート状正極（正極合剤層が形成されていない正極集電体５１、５１）であり、巻回中心部は、シート状負極（負極合剤層が形成されていない負極集電体６１、６１）である。   In the laminated battery 1 shown in FIG. 4, the sheet-like positive electrode 5 has a positive electrode mixture layer formed on one side or both sides of the current collector, and an end portion in the width direction of the current collector (the right end side in FIG. 4). ) To form a positive electrode tab without forming the positive electrode mixture layer, and the positive electrode tab is divided into a plurality of sets in the substantially oval flat portion of the wound electrode body to form the positive electrode tab laminates 5a and 5b. Yes. The positive electrode tab laminate 5a is connected to the positive electrode external terminal 3a, and the positive electrode tab laminate 5b is connected to the positive electrode external terminal 3b. Although not shown, in the laminated battery 1, the sheet-like negative electrode 6 has a negative electrode mixture layer formed on one side or both sides of the current collector and the side of the current collector opposite to the positive electrode tab The negative electrode mixture layer is not formed at the end portion (the left end portion in the figure) and becomes a negative electrode tab, and the negative electrode tab is divided into a plurality of groups in a substantially oval flat portion of the wound electrode body. The negative electrode tab laminate is formed. Each negative electrode tab laminate is connected to a different negative external terminal. In the wound electrode body according to the battery shown in FIG. 4, the outermost peripheral portion is a sheet-like positive electrode (positive electrode current collectors 51 and 51 in which a positive electrode mixture layer is not formed), and the winding center portion is It is a sheet-like negative electrode (negative electrode current collectors 61 and 61 in which a negative electrode mixture layer is not formed).

本発明のラミネート形電池では、巻回電極体を有する態様においては、かかる巻回電極体における巻回数が１０以上であり、この場合にも、積層数の多い積層電極体を有する電池の場合における前記の問題と同じ問題が起こり得る。そこで、巻回電極体を有する本発明の電池では、シート状正極の正極タブを積層した正極タブ積層体を複数に分け、各正極タブ積層体を、それぞれ別の正極外部端子に接続し、各正極外部端子をラミネートフィルム外装体の内部および外部の少なくとも一方で互いに電気的に接続している。また、図示していないが、巻回電極体を有する本発明の電池では、シート状負極についても、それらの負極タブを積層した負極タブ積層体を複数に分け、各負極タブ積層体を、それぞれ別の負極外部端子に接続し、各負極外部端子をラミネートフィルム外装体の内部および外部の少なくとも一方で互いに電気的に接続している。そのため、積層電極体を有する電池の場合と同様に、大電流放電を可能とし、かつ高い信頼性を確保しつつ、ラミネートフィルム外装体から外部端子を引き出す位置の自由度を高めることができる。   In the laminated battery of the present invention, in the embodiment having the wound electrode body, the number of turns in the wound electrode body is 10 or more, and also in this case, in the case of the battery having the laminated electrode body having a large number of layers. The same problem as above can occur. Therefore, in the battery of the present invention having a wound electrode body, the positive electrode tab laminate in which the positive electrode tabs of the sheet-like positive electrode are laminated is divided into a plurality, and each positive electrode tab laminate is connected to a separate positive electrode external terminal, The positive external terminal is electrically connected to at least one of the inside and the outside of the laminate film outer package. Although not shown, in the battery of the present invention having a wound electrode body, the sheet-like negative electrode is also divided into a plurality of negative electrode tab laminates in which those negative electrode tabs are laminated, It connects to another negative electrode external terminal, and each negative electrode external terminal is electrically connected to each other at least one of the inside and the outside of the laminate film exterior body. Therefore, as in the case of a battery having a laminated electrode body, it is possible to discharge a large current and to increase the degree of freedom in the position of drawing out an external terminal from the laminate film exterior body while ensuring high reliability.

なお、巻回電極体を有する本発明のラミネート形電池において、正極タブ積層体および負極タブ積層体の数は、積層電極体を有する場合と同様に、複数であればよく、少なくとも２以上であるが、通常は５以下であり、４以下であることが好ましく、３以下であることがより好ましい。また、１つの正極タブ積層体における正極タブの積層数は、５〜６０であることが好ましく、１つの負極タブ積層体における負極タブの積層数は、５〜６０であることが好ましい。   In the laminated battery of the present invention having a wound electrode body, the number of positive electrode tab laminates and negative electrode tab laminates may be plural as in the case of having a laminated electrode body, and is at least 2 or more. However, it is usually 5 or less, preferably 4 or less, and more preferably 3 or less. Moreover, it is preferable that the lamination | stacking number of the positive electrode tab in one positive electrode tab laminated body is 5-60, and it is preferable that the lamination | stacking number of the negative electrode tab in one negative electrode tab laminated body is 5-60.

なお、ラミネート形電池における複数の正極外部端子同士、および複数の負極外部端子同士を互いに電気的に接続するにあたっては、図３や図４に示すようにラミネートフィルム外装体の内部で重ねる方法（ただし、図３および図４では、外部でも重ねられている）が好ましいが、他にも、例えば、ラミネートフィルム外装体の外部でのみ重ねるなどして電気的に接続してもよい。また、複数の正極外部端子および複数の負極外部端子を、それぞれ重ねることなく平面視で横に並べるように配置し、ラミネートフィルム外装体の内部および外部の少なくとも一方で、リード体などを介して各正極外部端子および各負極外部端子を互いに電気的に接続してもよい。   In addition, in electrically connecting the plurality of positive electrode external terminals and the plurality of negative electrode external terminals to each other in the laminated battery, a method of superimposing them inside the laminate film outer package as shown in FIGS. 3 and 4 (however, In FIGS. 3 and 4, it is preferable that the layers are overlapped also on the outside. However, in addition, for example, they may be electrically connected by overlapping only on the outside of the laminate film outer package. In addition, a plurality of positive external terminals and a plurality of negative external terminals are arranged so as to be arranged side by side in a plan view without overlapping each other, and at least one of the inside and the outside of the laminate film exterior body, The positive external terminal and each negative external terminal may be electrically connected to each other.

更に、ラミネート形電池における正極外部端子と負極外部端子とは、ラミネートフィルム外装体の外周辺のうち、それぞれ別の辺から外部に取り出されていてもよいが、重ねられた複数の正極外部端子と、重ねられた複数の負極外部端子とが、ラミネートフィルム外装体の同じ辺から外部に引き出されていてもよい。   Furthermore, the positive electrode external terminal and the negative electrode external terminal in the laminated battery may be taken out from different sides of the outer periphery of the laminate film outer package, respectively, but a plurality of stacked positive electrode external terminals and The plurality of stacked negative electrode external terminals may be drawn to the outside from the same side of the laminate film outer package.

例えば、図３に示すような積層電極体を有する電池の場合には、図１に示すように、複数の正極外部端子が重ねられ、かつ複数の負極外部端子が重ねられており、これら重ねられた複数の正極外部端子と、重ねられた複数の負極外部端子とが、ラミネートフィルム外装体の同じ辺から外部に引き出されていることがより好ましく、この場合、ラミネートフィルム外装体の外周辺の熱シール部の体積を減らして、エネルギー密度をより高めるのに有利である。一方、図４に示すような巻回電極体を有する電池の場合には、電池の製造を容易にする観点からは、図２に示すように、重ねられた複数の正極外部端子と、重ねられた複数の負極外部端子とが、それぞれラミネートフィルム外装体の別の辺から外部に引き出されていることがより好ましく、四角形のラミネートフィルム外装体における重ねられた複数の正極外部端子が外部に引き出された辺と対向する辺から、重ねられた複数の負極外部端子が外部に引き出されていることが更に好ましい。   For example, in the case of a battery having a laminated electrode body as shown in FIG. 3, a plurality of positive external terminals are stacked and a plurality of negative external terminals are stacked as shown in FIG. More preferably, the plurality of positive electrode external terminals and the plurality of stacked negative electrode external terminals are drawn to the outside from the same side of the laminate film exterior body. It is advantageous to increase the energy density by reducing the volume of the seal portion. On the other hand, in the case of a battery having a wound electrode body as shown in FIG. 4, from the viewpoint of facilitating the manufacture of the battery, as shown in FIG. More preferably, the plurality of negative electrode external terminals are each drawn out from another side of the laminate film outer package, and the plurality of stacked positive electrode external terminals in the rectangular laminate film package are drawn out to the outside. More preferably, the plurality of stacked negative electrode external terminals are led out to the outside from the side facing the opposite side.

ラミネート形電池を構成するシート状正極は、例えば、正極活物質、導電助剤およびバインダなどを含有する正極合剤からなる層（正極合剤層）を、集電体の片面または両面に形成したものが使用できる。   In the sheet-like positive electrode constituting the laminate battery, for example, a layer made of a positive electrode mixture containing a positive electrode active material, a conductive additive and a binder (positive electrode mixture layer) is formed on one side or both sides of the current collector. Things can be used.

正極活物質としては、例えば、本発明のラミネート形電池がリチウムイオン二次電池の場合、リチウムイオンを吸蔵・放出できる活物質が使用される。このような正極活物質の具体例としては、例えば、Ｌｉ１＋ｘＭＯ２（−０．１＜ｘ＜０．１、Ｍ：Ｃｏ、Ｎｉ、Ｍｎ、Ａｌ、Ｍｇなど）で表される層状構造のリチウム含有遷移金属酸化物、ＬｉＭｎ２Ｏ４やその元素の一部を他元素で置換したスピネル構造のリチウムマンガン酸化物、ＬｉＭＰＯ４（Ｍ：Ｃｏ、Ｎｉ、Ｍｎ、Ｆｅなど）で表されるオリビン型化合物などが挙げられる。前記層状構造のリチウム含有遷移金属酸化物の具体例としては、ＬｉＣｏＯ２やＬｉＮｉ１−ｘＣｏｘ−ｙＡｌｙＯ２（０．１≦ｘ≦０．３、０．０１≦ｙ≦０．２）などの他、少なくともＣｏ、ＮｉおよびＭｎを含む酸化物（ＬｉＭｎ１／３Ｎｉ１／３Ｃｏ１／３Ｏ２、ＬｉＭｎ５／１２Ｎｉ５／１２Ｃｏ１／６Ｏ２、ＬｉＮｉ３／５Ｍｎ１／５Ｃｏ１／５Ｏ２など）などを例示することができる。 As the positive electrode active material, for example, when the laminate type battery of the present invention is a lithium ion secondary battery, an active material capable of inserting and extracting lithium ions is used. As a specific example of such a positive electrode active material, for example, a layered structure represented by Li 1 + x MO 2 (−0.1 <x <0.1, M: Co, Ni, Mn, Al, Mg, etc.) Lithium-containing transition metal oxide, LiMn 2 O 4 and spinel-structured lithium manganese oxide obtained by substituting some of its elements with other elements, LiMPO 4 (M: Co, Ni, Mn, Fe, etc.) Type compounds. Specific examples of the lithium-containing transition metal oxide having a layered structure include LiCoO 2 and LiNi 1-x Co xy Al y O 2 (0.1 ≦ x ≦ 0.3, 0.01 ≦ y ≦ 0. 2) and other oxides containing at least Co, Ni and Mn (LiMn 1/3 Ni 1/3 Co 1/3 O 2 , LiMn 5/12 Ni 5/12 Co 1/6 O 2 , LiNi 3 / 5 Mn 1/5 Co 1/5 O 2 etc.).

正極の集電体としては、アルミニウム箔やアルミニウム合金箔が好適である。集電体の厚みは、電池の大きさや容量にもよるが、例えば、０．０１〜０．０２ｍｍであることが好ましい。   As the current collector for the positive electrode, an aluminum foil or an aluminum alloy foil is suitable. The thickness of the current collector is preferably 0.01 to 0.02 mm, for example, although it depends on the size and capacity of the battery.

正極を作製するにあたっては、前記の正極活物質と、黒鉛、アセチレンブラック、カーボンブラック、繊維状炭素などの導電助剤と、ポリフッ化ビニリデン（ＰＶＤＦ）などのバインダなどを含む正極合剤を、Ｎ−メチル−２−ピロリドン（ＮＭＰ）などの溶剤を用いて均一に分散させたペースト状やスラリー状の組成物を調製し（バインダは、溶剤に溶解していてもよい）、この組成物を正極集電体上に塗布して乾燥し、必要に応じてプレス処理により正極合剤層の厚みや密度を調整する方法が採用できる。ただし、本発明に係る正極の作製方法は前記の方法に限られず、他の方法を採用しても構わない。   In producing the positive electrode, the positive electrode active material, a conductive additive such as graphite, acetylene black, carbon black, and fibrous carbon, and a positive electrode mixture containing a binder such as polyvinylidene fluoride (PVDF), N -A paste-like or slurry-like composition uniformly dispersed using a solvent such as methyl-2-pyrrolidone (NMP) is prepared (the binder may be dissolved in the solvent), and this composition is used as the positive electrode A method of applying to the current collector and drying, and adjusting the thickness and density of the positive electrode mixture layer by pressing as necessary can be employed. However, the manufacturing method of the positive electrode according to the present invention is not limited to the above method, and other methods may be adopted.

シート状正極における正極合剤層の厚みは、片面あたり、３０〜１００μｍとすることが好ましい。また、正極合剤層における各構成成分の含有量は、正極活物質：９０〜９８質量％、導電助剤：１〜５質量％、バインダ：１〜５質量％とすることが好ましい。   The thickness of the positive electrode mixture layer in the sheet-like positive electrode is preferably 30 to 100 μm per side. Moreover, it is preferable that content of each structural component in a positive mix layer shall be positive electrode active material: 90-98 mass%, conductive support agent: 1-5 mass%, and binder: 1-5 mass%.

正極外部端子には、使用機器との接続の容易さなどの関係から、アルミニウムまたはアルミニウム合金製のものを用いることが好ましい。正極外部端子の厚み（１枚あたりの厚み）は、５０μｍ以上が好適である。すなわち、正極外部端子の厚みを５０μｍ以上にすることによって、正極外部端子溶接時の切断の防止、並びに引っ張りおよび折り曲げによる断裂の防止を図ることができる。また、正極外部端子は、その総厚み（全正極外部端子の合計厚み）が６００μｍ以下であることが好ましく、これにより、ラミネートフィルム外装体の熱シール部に厚み方向の隙間が生じるのを防止することができる。   The positive electrode external terminal is preferably made of aluminum or an aluminum alloy from the viewpoint of ease of connection with the equipment used. The thickness of the positive electrode external terminal (thickness per sheet) is preferably 50 μm or more. That is, by setting the thickness of the positive external terminal to 50 μm or more, it is possible to prevent cutting during welding of the positive external terminal and to prevent tearing due to pulling and bending. Further, the positive electrode external terminal preferably has a total thickness (total thickness of all the positive electrode external terminals) of 600 μm or less, thereby preventing a gap in the thickness direction from being generated in the heat seal portion of the laminate film outer package. be able to.

なお、複数の正極外部端子同士は、図１から図４に示すように、それらの一部が接着層８を介して熱融着されていることが好ましい。よって、正極外部端子には、例えば、ラミネートフィルム外装体の熱シール部に位置することが予定されている箇所に、予め接着層を設けてもよい。なお、接着層としては、ラミネートフィルム外装体を構成する金属ラミネートフィルムが、電池内側となる面に有している熱融着樹脂層の構成樹脂（熱融着樹脂）と同種の樹脂を有するものが好ましい。   In addition, as shown in FIGS. 1 to 4, it is preferable that a part of the plurality of positive electrode external terminals is heat-sealed through the adhesive layer 8. Therefore, the positive electrode external terminal may be provided with an adhesive layer in advance, for example, at a place where it is planned to be located at the heat seal portion of the laminate film outer package. In addition, as a contact bonding layer, the metal laminate film which comprises a laminate film exterior body has the same kind of resin as the constituent resin (thermal fusion resin) of the thermal fusion resin layer which has on the surface which becomes a battery inner side Is preferred.

シート状正極と正極外部端子の接続は、シート状正極の集電体により構成される正極タブ（正極タブ積層体）と正極外部端子とを直接接続することで行ってもよいが、例えば、アルミニウム製のリード体を介してシート状正極の正極タブ（正極タブ積層体）と正極外部端子とを接続することで行うこともできる。アルミニウム製のリード体の厚みは、正極外部端子と同様に、５０〜３００μｍであることが好ましい。このようなリード体は、特に正極集電体であるアルミニウム箔が薄く、正極外部端子と直接接続するには強度が不足するような場合に用いることが好ましい。   The connection between the sheet-like positive electrode and the positive electrode external terminal may be performed by directly connecting the positive electrode tab (positive electrode tab laminate) constituted by the sheet-like positive electrode current collector and the positive electrode external terminal. It can also carry out by connecting the positive electrode tab (positive electrode tab laminated body) of a sheet-like positive electrode, and a positive electrode external terminal through the lead body made from a product. The thickness of the aluminum lead body is preferably 50 to 300 μm, like the positive external terminal. Such a lead body is preferably used when the aluminum foil as the positive electrode current collector is particularly thin and the strength is insufficient for direct connection with the positive electrode external terminal.

シート状正極における正極タブ（正極タブ積層体）または正極タブに接続したアルミニウム製のリード体と、正極外部端子との接続方法としては、例えば、抵抗溶接、超音波溶接、レーザー溶接、カシメ、導電性接着剤による方法など、各種の方法を採用することができるが、超音波溶接が特に適している。   Examples of the method of connecting the positive electrode tab (positive electrode tab laminate) in the sheet-like positive electrode or the aluminum lead body connected to the positive electrode tab and the positive electrode external terminal include resistance welding, ultrasonic welding, laser welding, caulking, conductive Various methods such as a method using an adhesive can be employed, but ultrasonic welding is particularly suitable.

ラミネート形電池を構成するシート状負極には、例えば、本発明のラミネート形電池がリチウムイオン二次電池の場合、リチウムイオンを吸蔵・放出できる活物質を含有するものが使用される。このような負極活物質としては、黒鉛、熱分解炭素類、コークス類、ガラス状炭素類、有機高分子化合物の焼成体、メソカーボンマイクロビーズ（ＭＣＭＢ）、炭素繊維などの、リチウムイオンを吸蔵、放出可能な炭素系材料の１種または２種以上の混合物が用いられる。また、Ｓｉ、Ｓｎ、Ｇｅ、Ｂｉ、Ｓｂ、Ｉｎなどの元素およびその合金、リチウム含有窒化物、または酸化物などのリチウム金属に近い低電圧で充放電できる化合物（ＬｉＴｉ５Ｏ１２など）、もしくはリチウム金属やリチウム／アルミニウム合金も負極活物質として用いることができる。これらの負極活物質に導電助剤（正極に係る導電助剤として例示した炭素材料など）やバインダ［ＰＶＤＦ、スチレンブタジエンゴム（ＳＢＲ）のようなゴム系バインダとカルボキシメチルセルロース（ＣＭＣ）との混合バインダなど］などを適宜添加した負極合剤を、集電体を芯材として成形体（負極合剤層）に仕上げたもの、または、前記の各種合金やリチウム金属の箔を集電体表面に積層したものなどが、シート状負極として用いられる。 As the sheet-like negative electrode constituting the laminated battery, for example, when the laminated battery of the present invention is a lithium ion secondary battery, one containing an active material capable of inserting and extracting lithium ions is used. Examples of such negative electrode active materials include graphite, pyrolytic carbons, cokes, glassy carbons, organic polymer compound fired bodies, mesocarbon microbeads (MCMB), and carbon fibers. One or a mixture of two or more releasable carbon-based materials is used. In addition, elements such as Si, Sn, Ge, Bi, Sb, In and their alloys, lithium-containing nitrides, or compounds that can be charged and discharged at a low voltage close to lithium metals such as oxides (such as LiTi 5 O 12 ), or Lithium metal or lithium / aluminum alloy can also be used as the negative electrode active material. These negative electrode active materials include conductive assistants (carbon materials exemplified as conductive assistants related to positive electrodes) and binders (mixed binders of rubber binders such as PVDF and styrene butadiene rubber (SBR) and carboxymethyl cellulose (CMC). Etc.] or the like, and a finished product (negative electrode mixture layer) using the current collector as a core material, or the above-mentioned various alloys and lithium metal foils are laminated on the surface of the current collector And the like are used as a sheet-like negative electrode.

例えば、負極合剤層を有するシート状負極とする場合、前記の負極活物質と前記のバインダと、必要に応じて黒鉛、アセチレンブラック、カーボンブラックなどの導電助剤などを含む負極合剤を、ＮＭＰなどの溶剤を用いて均一に分散させたペースト状やスラリー状の組成物を調製し（バインダは、溶剤に溶解していてもよい）、この組成物を負極集電体上に塗布して乾燥し、必要に応じてプレス処理により負極合剤層の厚みや密度を調整する方法が採用できる。ただし、本発明に係るシート状負極の作製方法は前記の方法に限られず、他の方法を採用しても構わない。   For example, in the case of a sheet-like negative electrode having a negative electrode mixture layer, a negative electrode mixture containing the negative electrode active material, the binder, and a conductive auxiliary agent such as graphite, acetylene black, and carbon black, if necessary, A paste-like or slurry-like composition uniformly dispersed using a solvent such as NMP is prepared (the binder may be dissolved in the solvent), and this composition is applied onto the negative electrode current collector. The method of drying and adjusting the thickness and density of a negative mix layer layer by press processing as needed can be employ | adopted. However, the method for producing the sheet-like negative electrode according to the present invention is not limited to the above method, and other methods may be adopted.

負極の集電体としては、銅箔が好適である。集電体の厚みは、電池の大きさや容量にもよるが、例えば、０．０５〜０．０２ｍｍであることが好ましい。   As the current collector for the negative electrode, a copper foil is suitable. The thickness of the current collector is preferably 0.05 to 0.02 mm, for example, although it depends on the size and capacity of the battery.

シート状負極における負極合剤層の厚みは、片面あたり、３０〜１００μｍとすることが好ましい。また、負極合剤層における各構成成分の含有量は、負極活物質：９０〜９８質量％、バインダ：１〜５質量％とすることが好ましい。また、負極に導電助剤を用いる場合には、負極合剤層中の導電助剤の含有量は、１〜５質量％とすることが好ましい。   The thickness of the negative electrode mixture layer in the sheet-like negative electrode is preferably 30 to 100 μm per side. Moreover, it is preferable that content of each structural component in a negative mix layer shall be negative electrode active material: 90-98 mass%, binder: 1-5 mass%. Moreover, when using a conductive support agent for a negative electrode, it is preferable that content of the conductive support agent in a negative mix layer shall be 1-5 mass%.

負極外部端子には、ニッケル、ニッケルメッキをした銅、ニッケル−銅クラッドなどの金属の板や箔、リボンなどが好ましい。また、負極外部端子の厚み（１枚あたりの厚み）は、正極外部端子と同様に５０μｍ以上であることが好ましい。すなわち、負極外部端子の厚みを５０μｍ以上にすることによって、負極外部端子溶接時の切断の防止、並びに引っ張りおよび折り曲げによる断裂の防止を図ることができる。また、ラミネートフィルム外装体の熱シール部に厚み方向の隙間が生じるのを防止するために、負極外部端子の総厚み（全負極外部端子の合計厚み）が６００μｍ以下であることが好ましい。   For the negative electrode external terminal, a metal plate such as nickel, nickel-plated copper, nickel-copper clad, foil, ribbon or the like is preferable. Moreover, it is preferable that the thickness (thickness per sheet) of the negative electrode external terminal is 50 μm or more like the positive electrode external terminal. That is, by setting the thickness of the negative electrode external terminal to 50 μm or more, it is possible to prevent cutting during welding of the negative electrode external terminal and to prevent tearing due to pulling and bending. Moreover, in order to prevent a gap in the thickness direction from being generated in the heat seal portion of the laminate film outer package, the total thickness of the negative electrode external terminals (total thickness of all the negative electrode external terminals) is preferably 600 μm or less.

なお、複数の負極外部端子同士は、正極外部端子の場合と同様に、図１および図２に示すように、それらの一部が接着層９を介して熱融着されていることが好ましい。よって、負極外部端子には、例えば、ラミネートフィルム外装体の熱シール部に位置することが予定されている箇所に、予め接着層を設けてもよい。なお、接着層としては、正極外部端子に係る接着層と同様に、ラミネートフィルム外装体を構成する金属ラミネートフィルムが、電池内側となる面に有している熱融着樹脂層の構成樹脂（熱融着樹脂）と同種の樹脂を有するものが好ましい。   As in the case of the positive electrode external terminal, a part of the plurality of negative electrode external terminals is preferably heat-sealed through the adhesive layer 9 as shown in FIGS. Therefore, the negative electrode external terminal may be provided with an adhesive layer in advance, for example, at a place where it is planned to be located at the heat seal portion of the laminate film outer package. As the adhesive layer, as in the adhesive layer relating to the positive electrode external terminal, the metal laminate film constituting the laminate film exterior body has a resin (heat Those having the same kind of resin as the fusion resin) are preferred.

シート状負極と負極外部端子の接続は、シート状負極の集電体により構成される負極タブ（負極タブ積層体）と負極外部端子とを直接接続することで行ってもよいが、例えば、銅製のリード体を介してシート状負極の負極タブ（負極タブ積層体）と負極外部端子とを接続することで行うこともできる。銅製のリード体の厚みは、負極外部端子と同様に、５０〜３００μｍであることが好ましい。このようなリード体は、特に負極集電体である銅箔が薄く、負極外部端子と直接接続するには強度が不足するような場合に用いることが好ましい。   The connection between the sheet-like negative electrode and the negative electrode external terminal may be performed by directly connecting the negative electrode tab (negative electrode tab laminate) constituted by the sheet-like negative electrode current collector and the negative electrode external terminal. It can also carry out by connecting the negative electrode tab (negative electrode tab laminated body) of a sheet-like negative electrode, and a negative electrode external terminal through the lead body of this. The thickness of the copper lead body is preferably 50 to 300 μm, similarly to the negative electrode external terminal. Such a lead body is preferably used when the copper foil as the negative electrode current collector is particularly thin and the strength is insufficient for direct connection with the negative electrode external terminal.

シート状負極における負極タブ（負極タブ積層体）または負極タブに接続した銅製のリード体との接続方法としては、例えば、抵抗溶接、超音波溶接、レーザー溶接、カシメ、導電性接着剤による方法など、各種の方法を採用することができるが、超音波溶接が特に適している。   Examples of the connection method with the negative electrode tab (negative electrode tab laminate) in the sheet-like negative electrode or the copper lead connected to the negative electrode tab include resistance welding, ultrasonic welding, laser welding, caulking, and a method using a conductive adhesive. Various methods can be employed, but ultrasonic welding is particularly suitable.

ラミネート形電池に係るセパレータとしては、例えば、ポリエチレン、ポリプロピレン、ポリエチレンとポリプロピレンの融合体、ポリエチレンテレフタレート、ポリブチレンテレフタレートなどで構成された多孔質フィルムや不織布が挙げられる。セパレータの厚みは１０〜５０μｍであることが好ましく、空孔率は３０〜７０％であることが好ましい。また、多孔質フィルムと不織布とを重ねるなど、複数枚のセパレータを用いることにより、短絡を防止する効果を高め、電池の信頼性をより向上させることができる。   Examples of the separator relating to the laminated battery include a porous film and a nonwoven fabric made of polyethylene, polypropylene, a fusion of polyethylene and polypropylene, polyethylene terephthalate, polybutylene terephthalate, and the like. The thickness of the separator is preferably 10 to 50 μm, and the porosity is preferably 30 to 70%. Moreover, the effect which prevents a short circuit can be improved and the reliability of a battery can be improved more by using several separators, such as overlapping a porous film and a nonwoven fabric.

ラミネート形電池に係る電解液としては、本発明のラミネート形電池がリチウムイオン二次電池の場合、例えば、エチレンカーボネート（ＥＣ）、プロピレンカーボネート（ＰＣ）、γ−ブチロラクトン（ＢＬ）などの高誘電率溶媒や、直鎖状の、ジメチルカーボネート（ＤＭＣ）、ジエチルカーボネート（ＤＥＣ）、メチルエチルカーボネート（ＥＭＣ）などの低粘度溶媒などの有機溶媒に、ＬｉＰＦ６、ＬｉＢＦ４などの溶質を溶解した溶液（非水電解液）が挙げられる。なお、電解液溶媒には、前記の高誘電率溶媒と、低粘度溶媒との混合溶媒を使用することがより好ましい。前記の溶液に、ＰＶＤＦやゴム系の材料、脂環エポキシやオキセタン系の三次元架橋構造を有する材料などを混合して固化し、ポリマー電解液としてもよい。 As an electrolyte solution for a laminate type battery, when the laminate type battery of the present invention is a lithium ion secondary battery, for example, a high dielectric constant such as ethylene carbonate (EC), propylene carbonate (PC), γ-butyrolactone (BL), etc. A solution in which a solute such as LiPF 6 or LiBF 4 is dissolved in a solvent or an organic solvent such as a linear solvent such as dimethyl carbonate (DMC), diethyl carbonate (DEC), or methyl ethyl carbonate (EMC). Non-aqueous electrolyte). In addition, it is more preferable to use the mixed solvent of the said high dielectric constant solvent and a low-viscosity solvent as an electrolyte solution solvent. PVDF, rubber-based material, alicyclic epoxy, oxetane-based material having a three-dimensional cross-linked structure, and the like may be mixed and solidified into the above solution to form a polymer electrolyte.

ラミネート形電池のラミネートフィルム外装体は、金属ラミネートフィルムで構成されたものであり、例えば、外装樹脂層／金属層／熱溶着性樹脂層からなる３層構造の金属ラミネートフィルムが挙げられる。金属ラミネートフィルムにおける外装樹脂層としては、ナイロンフィルム（ナイロン６６フィルムなど）、ポリエステルフィルム（ＰＥＴフィルムなど）などが、金属層としてはアルミニウムフィルム、ステンレス鋼フィルムなどが、熱溶着性樹脂層としては変性ポリオレフィンフィルム（変性ポリオレフィンアイオノマーフィルムなど）などが挙げられる。   The laminate film outer package of the laminate type battery is composed of a metal laminate film, and examples thereof include a metal laminate film having a three-layer structure including an outer resin layer / a metal layer / a heat-weldable resin layer. Nylon film (such as nylon 66 film), polyester film (such as PET film), etc. as the exterior resin layer in the metal laminate film, aluminum film, stainless steel film, etc. as the metal layer, modified as the heat-weldable resin layer Polyolefin film (modified polyolefin ionomer film etc.) etc. are mentioned.

金属ラミネートフィルムにおいては、外装樹脂層の厚みが２０〜１００μｍであることが好ましく、金属層の厚みが１０〜１５０μｍであることが好ましく、熱融着性樹脂層の厚みが２０〜１００μｍであることが好ましい。   In the metal laminate film, the thickness of the exterior resin layer is preferably 20 to 100 μm, the thickness of the metal layer is preferably 10 to 150 μm, and the thickness of the heat-fusible resin layer is 20 to 100 μm. Is preferred.

なお、ラミネートフィルム外装体は、平面視で多角形であれば、その形状については特に制限は無く、必要に応じて、平面視で、三角形、四角形、五角形、六角形、七角形、八角形などの各種形状を取り得るが、平面視で四角形（矩形または正方形）が一般的である。ただし、巻回電極体を有する電池の場合には、平面視で四角形のラミネートフィルム外装体を使用する。   In addition, if the laminate film exterior body is a polygon in plan view, the shape is not particularly limited, and if necessary, in a plan view, a triangle, a rectangle, a pentagon, a hexagon, a heptagon, an octagon, etc. However, it is generally a quadrangle (rectangle or square) in plan view. However, in the case of a battery having a wound electrode body, a rectangular laminate film exterior body is used in plan view.

本発明のラミネート形電池は、自動車用途などの高出力、高容量の電池が要求される用途を始めとして、各種電子機器の電源用途など、従来から知られているラミネート形電池（特にラミネート形のリチウムイオン二次電池）が使用されている各種用途と同様の用途に用いることができる。   The laminated battery of the present invention is a conventionally known laminated battery (especially a laminated battery) such as a power supply for various electronic devices, including applications requiring high output and high capacity batteries such as automobile applications. It can be used for the same applications as various applications in which lithium ion secondary batteries) are used.

以下、実施例に基づいて本発明を詳細に述べる。ただし、下記実施例は、本発明を制限するものではない。   Hereinafter, the present invention will be described in detail based on examples. However, the following examples do not limit the present invention.

実施例１
＜正極の作製＞
ＬｉＣｏＯ２：９６質量部、アセチレンブラック：２質量部、およびＰＶＤＦ：２質量部を混合し、更にＮＭＰを加えて正極合剤含有ペーストを調製した。得られた正極合剤含有ペーストを、厚みが１５μｍのアルミニウム箔からなる集電体の両面に塗布し、乾燥後、プレス処理を施して正極合剤層を形成し、シート状正極を得た。得られたシート状正極の正極合剤層の厚みは、集電体の片面あたり６０μｍであった。その後、得られたシート状正極を、正極合剤層の形成部分が幅１０５ｍｍ、長さ２００ｍｍとなり、更に正極タブとなる正極集電体の露出部も含む形状に裁断した。 Example 1
<Preparation of positive electrode>
LiCoO 2 : 96 parts by mass, acetylene black: 2 parts by mass, and PVDF: 2 parts by mass were mixed, and NMP was further added to prepare a positive electrode mixture-containing paste. The obtained positive electrode mixture-containing paste was applied to both sides of a current collector made of an aluminum foil having a thickness of 15 μm, dried, and then subjected to a press treatment to form a positive electrode mixture layer, whereby a sheet-like positive electrode was obtained. The thickness of the positive electrode mixture layer of the obtained sheet-like positive electrode was 60 μm per one side of the current collector. Thereafter, the obtained sheet-like positive electrode was cut into a shape in which a portion where the positive electrode mixture layer was formed had a width of 105 mm and a length of 200 mm, and also included an exposed portion of a positive electrode current collector that became a positive electrode tab.

＜負極の作製＞
黒鉛：９８質量％に、ＳＢＲ：１．５質量％およびＣＭＣ：０．５質量％を加えて混合し、更に水を加えて負極合剤含有ペーストを調製した。得られた負極合剤含有ペーストを、厚みが１０μｍの銅箔からなる集電体の両面に塗布し、乾燥後、プレス処理を施して負極合剤層を形成し、シート状負極を得た。得られたシート状負極の負極合剤層の厚みは、集電体の片面あたり６０μｍであった。その後、得られたシート状負極を、負極合剤層の形成部分が幅１１０ｍｍ、長さ２０５ｍｍとなり、更に負極タブとなる負極集電体の露出部も含む形状に裁断した。 <Production of negative electrode>
Graphite: 98% by mass, SBR: 1.5% by mass and CMC: 0.5% by mass were added and mixed, and further water was added to prepare a negative electrode mixture-containing paste. The obtained negative electrode mixture-containing paste was applied to both sides of a current collector made of a copper foil having a thickness of 10 μm, dried, and then subjected to a press treatment to form a negative electrode mixture layer, whereby a sheet-like negative electrode was obtained. The thickness of the negative electrode mixture layer of the obtained sheet-like negative electrode was 60 μm per one side of the current collector. Thereafter, the obtained sheet-like negative electrode was cut into a shape in which a portion where the negative electrode mixture layer was formed had a width of 110 mm and a length of 205 mm, and also included an exposed portion of a negative electrode current collector that became a negative electrode tab.

＜電池の組み立て＞
前記のシート状正極５０枚と、前記のシート状負極５１枚とを、セパレータ（厚みが２５μｍのポリオレフィン微孔性フィルム）を介して積層し、積層電極体とした。なお、積層電極体の両端は、いずれも負極となるように積層した。次に、前記の積層電極体に係る各シート状正極のうち、上側２５枚分の正極タブを重ねた正極タブ積層体を正極外部端子に超音波溶接し、下側２５枚分の正極タブを重ねた正極タブ積層体を、別の正極外部端子に超音波溶接した。また、前記の積層電極体に係る各シート状負極のうち、上側２５枚分の負極タブを重ねた負極タブ積層体を負極外部端子に超音波溶接し、下側２６枚分の負極タブを重ねた負極タブ積層体を別の負極外部端子に超音波溶接した。 <Battery assembly>
50 sheets of the sheet-like positive electrode and 51 sheets of the sheet-like negative electrode were laminated via a separator (a polyolefin microporous film having a thickness of 25 μm) to obtain a laminated electrode body. In addition, it laminated | stacked so that both ends of a laminated electrode body might become a negative electrode. Next, among each sheet-like positive electrode related to the above-mentioned laminated electrode body, the positive electrode tab laminate in which the positive electrode tabs for the upper 25 sheets are stacked is ultrasonically welded to the positive electrode external terminal, and the lower 25 positive electrode tabs are attached. The stacked positive electrode tab laminate was ultrasonically welded to another positive electrode external terminal. In addition, among the sheet-like negative electrodes related to the laminated electrode body, the negative electrode tab laminated body in which the negative electrode tabs for the upper 25 sheets are stacked is ultrasonically welded to the negative electrode external terminal, and the negative electrode tabs for the lower 26 sheets are stacked. The negative electrode tab laminate was ultrasonically welded to another negative electrode external terminal.

なお、正極外部端子には、長さ３０ｍｍ、幅２０ｍｍ、厚み０．２ｍｍのアルミニウム板を２枚用い、負極外部端子には、長さ３０ｍｍ、幅２０ｍｍ、厚み０．２ｍｍの銅板を２枚用いた。また、正極外部端子および負極外部端子には、ラミネートフィルム外装体の熱シール部に位置することが予定される箇所の両面に、ラミネートフィルム外装体の熱溶着性樹脂層を構成する樹脂と同じ変性ポリオレフィンにより構成された接着層を配した。   For the positive electrode external terminal, two aluminum plates with a length of 30 mm, a width of 20 mm, and a thickness of 0.2 mm are used. For the negative electrode external terminal, two copper plates with a length of 30 mm, a width of 20 mm, and a thickness of 0.2 mm are used. It was. In addition, the positive external terminal and the negative external terminal have the same modification as the resin constituting the heat-welding resin layer of the laminate film exterior body on both sides of the place where the heat seal portion of the laminate film exterior body is expected to be located. An adhesive layer made of polyolefin was disposed.

ポリエステルフィルム／アルミニウムフィルム／変性ポリオレフィンフィルムからなる厚み１５０μｍの三層構造の金属ラミネートフィルム（矩形で、サイズ１３０ｍｍ×２３０ｍｍ）を２枚用意した。そして、一方の金属ラミネートフィルムにおける変性ポリオレフィンフィルム層上に前記の積層電極体を、複数の正極外部端子を重ねたものの一部および複数の負極外部端子を重ねたものの一部が、図１に示すように金属ラミネートフィルムの同一辺から突出するように置き、その上にもう一方の金属ラミネートフィルムを重ねて、３辺を熱シールしてラミネートフィルム外装体とし、７０℃で１５時間真空乾燥した。その後、ラミネートフィルム外装体の封止していない一辺から非水電解液を注入し、減圧状態で前記の一辺を熱シールして、ラミネート形リチウムイオン二次電池とした。なお、非水電解液には、ＥＣとＤＥＣを体積比で１対３に混合した溶媒にＬｉＰＦ６を濃度１．０ｍｏｌ／ｌで溶解した溶液を用いた。また、ラミネートフィルム外装体の熱シールの幅は、１０ｍｍとした。 Two sheets of a 150-μm thick three-layered metal laminate film (rectangular, size 130 mm × 230 mm) made of polyester film / aluminum film / modified polyolefin film were prepared. FIG. 1 shows a part of the laminated electrode body on the modified polyolefin film layer of one metal laminate film, a part of the plurality of positive external terminals stacked and a part of the plurality of negative external terminals stacked. The other side of the metal laminate film was placed so as to protrude from the same side of the metal laminate film, and the other side of the metal laminate film was stacked thereon. The three sides were heat-sealed to form a laminate film outer package, which was vacuum dried at 70 ° C. for 15 hours. Thereafter, a non-aqueous electrolyte was injected from one side of the laminate film outer package that was not sealed, and the one side was heat-sealed under reduced pressure to obtain a laminated lithium ion secondary battery. Note that the nonaqueous electrolytic solution, a solution was used in which a LiPF 6 in a solvent mixture to 1: 3 to EC and DEC at a volume ratio at a concentration 1.0 mol / l. The width of the heat seal of the laminate film outer package was 10 mm.

前記のラミネート形リチウムイオン二次電池について、２４時間エージングし、その後、０．１Ｃの電流値で１時間充電し、続いて総充電時間を４時間とする定電流−定電圧充電（定電流充電：０．５Ｃ、定電圧充電：４．２Ｖ）を実施することで化成処理を行った。   The laminated lithium ion secondary battery is aged for 24 hours, then charged with a current value of 0.1 C for 1 hour, and then a constant current-constant voltage charge (constant current charge) with a total charge time of 4 hours. : 0.5C, constant voltage charging: 4.2V), the chemical conversion treatment was performed.

実施例２
実施例１と同様にして正極集電体の両面に正極合剤層を形成し、幅が２００ｍｍで、その幅方向の片端に正極タブとなる正極集電体の露出部を有し、かつ長尺方向の両端にも正極集電体の露出部を有する長尺（長さ６ｍ）のシート状正極を作製した。また、実施例２と同様にして負極集電体の両面に負極合剤層を形成し、幅が２０５ｍｍで、その幅方向の片端に負極タブとなる負極集電体の露出部を有し、かつ長尺方向の両端にも負極集電体の露出部を有する長尺（長さ６．１ｍ）のシート状負極を作製した。 Example 2
In the same manner as in Example 1, a positive electrode mixture layer was formed on both surfaces of the positive electrode current collector, had a width of 200 mm, had an exposed portion of the positive electrode current collector serving as a positive electrode tab at one end in the width direction, and was long A long (6 m long) sheet-like positive electrode having exposed portions of the positive electrode current collector at both ends in the scale direction was produced. Further, in the same manner as in Example 2, a negative electrode mixture layer was formed on both surfaces of the negative electrode current collector, the width was 205 mm, and the exposed portion of the negative electrode current collector serving as a negative electrode tab was formed at one end in the width direction. In addition, a long (length: 6.1 m) sheet-like negative electrode having an exposed portion of the negative electrode current collector at both ends in the long direction was produced.

前記のシート状正極と前記のシート状負極とを、セパレータ（厚みが２５μｍのポリオレフィン微孔性フィルム）介し、かつシート状正極に係る正極タブとシート状負極に係る負極タブとが、それぞれ電極体の別の端面側となるように重ね合わせて渦巻き状に巻回し（巻回数２５回）、押し潰して横断面が略長円形の巻回電極体とした。次に、巻回電極体に係るシート状正極の正極タブのうち、横断面における長軸を挟んで一方の正極タブ２５枚を短軸方向に重ねた正極タブ積層体を正極外部端子に超音波溶接し、他方の正極タブ２５枚分を短軸方向に重ねた正極タブ積層体を、別の正極外部端子に超音波溶接した。また、巻回電極体に係るシート状負極の負極タブのうち、横断面における長軸を挟んで一方の負極タブ２５枚分を短軸方向に重ねた負極タブ積層体を負極外部端子に超音波溶接し、他方の負極タブ２６枚分を短軸方向に重ねた負極タブ積層体を別の負極外部端子に超音波溶接した。   The sheet-like positive electrode and the sheet-like negative electrode are passed through a separator (polyolefin microporous film having a thickness of 25 μm), and the positive electrode tab relating to the sheet-like positive electrode and the negative electrode tab relating to the sheet-like negative electrode are respectively electrode bodies. These were stacked so as to be on the other end face side, wound into a spiral shape (number of windings: 25), and crushed to obtain a wound electrode body having a substantially oval cross section. Next, among the positive electrode tabs of the sheet-like positive electrode related to the wound electrode body, a positive electrode tab laminate in which one positive electrode tab is stacked in the short axis direction across the major axis in the cross section is ultrasonically applied to the positive electrode external terminal. The positive electrode tab laminate in which the other 25 positive electrode tabs were stacked in the minor axis direction was welded ultrasonically to another positive electrode external terminal. In addition, among the negative electrode tabs of the sheet-like negative electrode related to the wound electrode body, the negative electrode tab laminated body in which one negative electrode tab of 25 sheets is stacked in the short axis direction across the major axis in the cross section is ultrasonically applied to the negative electrode external terminal. Welding was performed, and a negative electrode tab laminate in which the other 26 negative electrode tabs were stacked in the minor axis direction was ultrasonically welded to another negative electrode external terminal.

なお、正極外部端子および負極外部端子には、実施例１と同じものを用い、ラミネートフィルム外装体の熱シール部に位置することが予定される箇所の両面に、ラミネートフィルム外装体の熱溶着性樹脂層を構成する樹脂と同じ変性ポリオレフィンにより構成された接着層を配した。   In addition, the same thing as Example 1 is used for a positive electrode external terminal and a negative electrode external terminal, and the heat-weldability of a laminate film exterior body is provided on both surfaces of the place where it is planned to be located in the heat seal part of a laminate film exterior body. An adhesive layer made of the same modified polyolefin as the resin constituting the resin layer was disposed.

前記の巻回電極体を積層電極体に代えて用い、正負極の外部端子の引き出し位置を図２に示すようにした以外は、実施例１と同様にしてラミネート形リチウムイオン二次電池を作製した。   A laminated lithium ion secondary battery is produced in the same manner as in Example 1 except that the above-described wound electrode body is used in place of the laminated electrode body and the lead-out positions of the positive and negative external terminals are as shown in FIG. did.

実施例３
正極外部端子および負極外部端子におけるラミネートフィルム外装体の熱シール部に位置することが予定される箇所の両面に、ラミネートフィルム外装体の熱溶着性樹脂層を構成する樹脂と同じ変性ポリオレフィンにより構成された接着層を配しなかった以外は、実施例１と同様にしてラミネート形リチウムイオン二次電池を作製した。 Example 3
It is composed of the same modified polyolefin as the resin constituting the heat-welding resin layer of the laminate film exterior body on both surfaces of the positive electrode external terminal and the negative electrode external terminal that are supposed to be located in the heat seal portion of the laminate film exterior body. A laminated lithium ion secondary battery was produced in the same manner as in Example 1 except that no adhesive layer was provided.

比較例１
全シート状正極５０枚の正極タブを重ねて１つの正極タブ積層体とし、これを１つの正極外部端子に超音波溶接し、また、全シート状負極５１枚の負極タブを重ねて１つの負極タブ積層体とし、これを１つの負極外部端子に超音波溶接した以外は、実施例１と同様にしてラミネート形リチウムイオン二次電池を作製した。 Comparative Example 1
The positive tabs of 50 sheets of all sheet-like positive electrodes are stacked to form one positive electrode tab laminate, which is ultrasonically welded to one positive electrode external terminal, and the negative tabs of 51 sheets of all-sheet negative electrodes are stacked to form one negative electrode. A laminated lithium ion secondary battery was produced in the same manner as in Example 1 except that a tab laminate was formed and this was ultrasonically welded to one negative electrode external terminal.

比較例２
巻回電極体に係るシート状正極の正極タブのうち、横断面における長軸を挟んで一方の正極タブ２５枚を短軸方向に重ねた正極タブ積層体と、他方の正極タブ２５枚分を短軸方向に重ねた正極タブ積層体とを、１つの正極外部端子のそれぞれ別の面に配して超音波溶接し、また、巻回電極体に係るシート状負極の負極タブのうち、横断面における長軸を挟んで一方の負極タブ２５枚分を短軸方向に重ねた負極タブ積層体と、他方の負極タブ２６枚分を短軸方向に重ねた負極タブ積層体とを、１つの負極外部端子のそれぞれ別の面に配して超音波溶接した以外は、実施例１と同様にしてラミネート形リチウムイオン二次電池を作製した。 Comparative Example 2
Among the positive electrode tabs of the sheet-like positive electrode related to the wound electrode body, a positive electrode tab laminate in which one positive electrode tab 25 is stacked in the short axis direction across the major axis in the cross section, and the other positive electrode tab 25 pieces The positive electrode tab laminate stacked in the minor axis direction is arranged on each of the other surfaces of one positive electrode external terminal and ultrasonically welded, and the negative electrode tab of the sheet-like negative electrode related to the wound electrode body is crossed. A negative electrode tab laminate in which one negative tab 25 is stacked in the short axis direction with a major axis on the surface sandwiched, and a negative electrode tab stack in which the other 26 negative tabs are stacked in the short axis direction A laminated lithium ion secondary battery was produced in the same manner as in Example 1 except that ultrasonic welding was performed by placing the electrodes on different surfaces of the negative electrode external terminal.

比較例３
正極外部端子の長さを４０ｍｍに変更し、巻回電極体に係るシート状正極の正極タブのうち、横断面における長軸を挟んで一方の正極タブ２５枚を短軸方向に重ねた正極タブ積層体と、他方の正極タブ２５枚分を短軸方向に重ねた正極タブ積層体とを、それぞれ１つの正極外部端子の別の位置に超音波溶接し、また、負極外部端子の長さを４０ｍｍに変更し、巻回電極体に係るシート状負極の負極タブのうち、横断面における長軸を挟んで一方の負極タブ２５枚分を短軸方向に重ねた負極タブ積層体と、他方の負極タブ２６枚分を短軸方向に重ねた負極タブ積層体とを、それぞれ１つの負極外部端子の別の位置に超音波溶接し、ラミネートフィルム外装体を構成する金属ラミネートフィルムのサイズを１３０ｍｍ×２４０ｍｍに変更した以外は、実施例２と同様にしてラミネート形リチウムイオン二次電池を作製した。 Comparative Example 3
A positive electrode tab in which the length of the positive electrode external terminal is changed to 40 mm, and one of the positive electrode tabs of the sheet-like positive electrode related to the wound electrode body is stacked with 25 positive electrode tabs in the short axis direction across the long axis in the cross section. The laminate and the positive electrode tab laminate in which the other 25 positive electrode tabs are stacked in the minor axis direction are ultrasonically welded to different positions of one positive external terminal, and the length of the negative external terminal is Of the negative electrode tabs of the sheet-like negative electrode related to the wound electrode body, the negative electrode tab laminated body in which 25 pieces of one negative electrode tab are stacked in the short axis direction across the major axis in the cross section, and the other The negative electrode tab laminate in which the 26 negative electrode tabs are stacked in the minor axis direction is ultrasonically welded to another position of each negative electrode external terminal, and the size of the metal laminate film constituting the laminate film exterior body is 130 mm × Other than changing to 240mm , To produce a laminate type lithium ion secondary battery in the same manner as in Example 2.

実施例１〜３および比較例１〜３のラミネート形リチウムイオン二次電池について、正極タブ積層体の正極外部端子への溶接時、および負極タブ積層体の負極外部端子への溶接時の状況（溶接信頼性）を評価した。また、実施例１〜３および比較例１〜３のラミネート形リチウムイオン二次電池について、下記の各評価を行った。積層電極体を有する実施例１、３および比較例１の電池の評価結果を表１に、巻回電極体を有する実施例２および比較例２、３の電池の評価結果を表２に、それぞれ示す。   About the laminated lithium ion secondary batteries of Examples 1 to 3 and Comparative Examples 1 to 3, the situation when welding the positive electrode tab laminate to the positive electrode external terminal and the welding of the negative electrode tab laminate to the negative electrode external terminal ( Welding reliability) was evaluated. In addition, the following evaluations were performed on the laminated lithium ion secondary batteries of Examples 1 to 3 and Comparative Examples 1 to 3. The evaluation results of the batteries of Examples 1 and 3 and Comparative Example 1 having a laminated electrode body are shown in Table 1, the evaluation results of the batteries of Example 2 and Comparative Examples 2 and 3 having a wound electrode body are shown in Table 2, respectively. Show.

＜内部抵抗＞
各電池の内部抵抗を、交流インピーダンス測定（１ｋＨｚ）により求めた。 <Internal resistance>
The internal resistance of each battery was determined by AC impedance measurement (1 kHz).

＜振動試験後の内部抵抗＞
各電池について、ＪＩＳ Ｃ ８７１２の４．２．２の規定に準拠した振動試験を行い、その後に各電池の内部抵抗を、交流インピーダンス測定（１ｋＨｚ）により求めた。 <Internal resistance after vibration test>
Each battery was subjected to a vibration test in accordance with the provisions of 4.2.2 of JIS C 8712. Thereafter, the internal resistance of each battery was determined by AC impedance measurement (1 kHz).

＜貯蔵後の内部抵抗＞
各電池について、６０℃、相対湿度９０％の環境下で２０日貯蔵した後の内部抵抗を、交流インピーダンス測定（１ｋＨｚ）により求めた。 <Internal resistance after storage>
For each battery, the internal resistance after storage for 20 days in an environment of 60 ° C. and 90% relative humidity was determined by AC impedance measurement (1 kHz).

Figure 2012212506
Figure 2012212506

表１から明らかなように、正極タブ積層体および負極タブ積層体を複数に分け、それぞれ別の外部端子に溶接した実施例１、３の電池では、正極タブ積層体および負極タブ積層体と、正負極の外部端子とが良好に溶接できており、各条件下での内部抵抗も小さく、高い信頼性を有している。これに対し、全ての正極タブおよび負極タブを、それぞれ１つの積層体とし、これら正極タブ積層体および負極タブ積層体を、それぞれ１つの外部端子に溶接した比較例１の電池では、タブの積層数が非常に多いことから、十分な溶接強度を確保するために、より厳しい条件で溶接する必要があり、全てのタブが良好に溶接できる条件とした結果、タブの溶接点近傍に割れやひびが生じて内部抵抗が高くなり、信頼性が乏しい。また、その比較例１の電池における溶接信頼性の影響は、電池に振動試験を行うと一層顕著となり、その後の内部抵抗が大きく増大しており、集電が十分に行われていないことが分かる。   As is clear from Table 1, in the batteries of Examples 1 and 3 in which the positive electrode tab laminate and the negative electrode tab laminate were divided into a plurality of parts and welded to different external terminals, the positive electrode tab laminate and the negative electrode tab laminate, The positive and negative external terminals are well welded, the internal resistance under each condition is small, and high reliability is achieved. On the other hand, in the battery of Comparative Example 1 in which all the positive electrode tabs and the negative electrode tabs are each formed as a single laminate, and the positive electrode tab laminate and the negative electrode tab laminate are each welded to one external terminal, Since the number is very large, it is necessary to weld under more severe conditions in order to ensure sufficient welding strength, and as a result that all tabs can be welded satisfactorily, there are cracks and cracks near the welding point of the tabs. The internal resistance becomes high and reliability is poor. Moreover, the influence of the welding reliability in the battery of Comparative Example 1 becomes more prominent when the battery is subjected to a vibration test, the internal resistance thereafter increases greatly, and it can be seen that current collection is not sufficiently performed. .

なお、実施例１の電池では、２枚の正極外部端子間、および２枚の負極外部端子間に接着層を配しているのに対し、実施例３の電池では、接着層を配していない。これらの電池では、作製後の内部抵抗に違いはないが、過酷な条件下で貯蔵した後には、実施例１の電池の方が内部抵抗の増大が小さく、ラミネートフィルム外装体の封止信頼性が向上していることが認められる。このように、複数の外部端子間に接着層を配することで、接着層によるコストの増大や、製造工程の増加があるものの、電池の信頼性を更に高めることができる。   In the battery of Example 1, an adhesive layer is disposed between the two positive external terminals and between the two negative external terminals, whereas in the battery of Example 3, the adhesive layer is disposed. Absent. In these batteries, there is no difference in the internal resistance after fabrication, but after storage under severe conditions, the battery of Example 1 has a smaller increase in internal resistance and the sealing reliability of the laminate film outer package. Is seen to be improved. As described above, by disposing the adhesive layer between the plurality of external terminals, the reliability of the battery can be further enhanced although there is an increase in cost due to the adhesive layer and an increase in the manufacturing process.

Figure 2012212506
Figure 2012212506

表２から明らかなように、巻回電極体を用いた実施例２の電池でも、積層電極体を用いた実施例１、３の電池と同様に、正極タブ積層体および負極タブ積層体と、正負極の外部端子とが良好に溶接できており、各条件下での内部抵抗も小さく、高い信頼性を有している。これに対し、全ての正極タブおよび負極タブを、それぞれ１つの外部端子に溶接した比較例２の電池では、積層電極体を用いた比較例１の電池と同様に、全てのタブが良好に溶接できる条件とした結果、タブの溶接点近傍に割れやひびが生じて内部抵抗が高くなり、信頼性が乏しい。   As is clear from Table 2, the battery of Example 2 using the wound electrode body was also the same as the batteries of Examples 1 and 3 using the laminated electrode body, and the positive electrode tab laminate and the negative electrode tab laminate, The positive and negative external terminals are well welded, the internal resistance under each condition is small, and high reliability is achieved. On the other hand, in the battery of Comparative Example 2 in which all the positive electrode tabs and negative electrode tabs were welded to one external terminal, all the tabs were well welded in the same manner as the battery of Comparative Example 1 using the laminated electrode body. As a result of being able to do so, cracks and cracks occur near the weld point of the tab, resulting in high internal resistance and poor reliability.

また、長い正極外部端子を使用し、２つに分けた正極タブ積層体を、それぞれ１つの正極外部端子の別の箇所に溶接し、かつ長い負極外部端子を使用し、２つに分けた負極タブ積層体を、それぞれ１つの負極外部端子の別の箇所に溶接した比較例３の電池でも、正極タブ積層体および負極タブ積層体と、正負極の外部端子とを、それぞれ２度にわたって溶接した結果、２回目の溶接の際に、最初に溶接したタブの溶接点近傍に割れやひびが生じ、信頼性が低下した。また、正負極の外部端子を長くし、より多くの溶接箇所を取る必要があったために電池の体積が増大し、更に、外部端子の配置の自由度が低下した。また、集電部分の抵抗も、正負極のタブ、外部端子ともに長くなることで増大した。   Also, using a long positive external terminal, the positive electrode tab laminate divided into two parts is welded to another part of one positive external terminal, and the negative electrode divided into two using a long negative external terminal Even in the battery of Comparative Example 3 in which the tab laminate was welded to another part of one negative electrode external terminal, the positive electrode tab laminate, the negative electrode tab laminate, and the positive and negative external terminals were welded twice each. As a result, during the second welding, cracks and cracks occurred in the vicinity of the weld point of the first welded tab, and the reliability decreased. In addition, since the positive and negative external terminals have to be lengthened and more welding points have to be taken, the volume of the battery is increased, and the degree of freedom in arranging the external terminals is further reduced. In addition, the resistance of the current collecting portion also increased as both the positive and negative electrode tabs and the external terminals became longer.

１ ラミネート形電池
２ ラミネートフィルム外装体
３ａ，３ｂ 正極外部端子
４ａ 負極外部端子
５ シート状正極
５ａ，５ｂ 正極タブ積層体
６ シート状負極 DESCRIPTION OF SYMBOLS 1 Laminated battery 2 Laminate film exterior body 3a, 3b Positive electrode external terminal 4a Negative electrode external terminal 5 Sheet-like positive electrode 5a, 5b Positive electrode tab laminated body 6 Sheet-like negative electrode

Claims (5)

集電体の少なくとも片面に正極合剤層を有する複数のシート状正極と集電体の少なくとも片面に負極合剤層を有する複数のシート状負極とがセパレータを介して積層された積層電極体が、平面視で多角形のラミネートフィルム外装体に収容されており、前記ラミネートフィルム外装体の外周辺が熱シールされているラミネート形電池であって、
前記積層電極体の有するシート状正極とシート状負極との合計数が２０以上であり、
各シート状正極の集電体の一部は、正極合剤層が形成されずに正極タブとされ、
各シート状負極の集電体の一部は、負極合剤層が形成されずに負極タブとされ、
前記複数のシート状正極の正極タブが、複数の組に分けられて積層されることにより、複数の正極タブ積層体が形成されており、
前記複数のシート状負極の負極タブが、複数の組に分けられて積層されることにより、複数の負極タブ積層体が形成されており、
各正極タブ積層体は、それぞれ別の正極外部端子に接続され、かつ各負極タブ積層体は、それぞれ別の負極外部端子に接続されており、
各正極外部端子および各負極外部端子は、それぞれラミネートフィルム外装体の内部または外部の少なくとも一方で互いに電気的に接続されていることを特徴とするラミネート形電池。 A laminated electrode body in which a plurality of sheet-like positive electrodes having a positive electrode mixture layer on at least one side of a current collector and a plurality of sheet-like negative electrodes having a negative electrode mixture layer on at least one side of the current collector are laminated via a separator. A laminated battery that is accommodated in a polygonal laminate film outer package in plan view, and the outer periphery of the laminate film outer package is heat-sealed,
The total number of the sheet-like positive electrode and the sheet-like negative electrode of the laminated electrode body is 20 or more,
A part of the collector of each sheet-like positive electrode is a positive electrode tab without forming a positive electrode mixture layer,
A part of the collector of each sheet-like negative electrode is a negative electrode tab without forming a negative electrode mixture layer,
The positive electrode tabs of the plurality of sheet-like positive electrodes are divided into a plurality of groups and stacked, thereby forming a plurality of positive electrode tab laminates,
The negative electrode tabs of the plurality of sheet-like negative electrodes are divided into a plurality of sets and stacked, thereby forming a plurality of negative electrode tab laminates,
Each positive electrode tab laminate is connected to a separate positive external terminal, and each negative tab laminate is connected to a separate negative external terminal,
Each positive electrode external terminal and each negative electrode external terminal are electrically connected to each other at least either inside or outside the laminate film outer package. 各正極タブ積層体と接続されたそれぞれの正極外部端子がラミネートフィルム外装体の内部で重ねられ、かつ各負極タブ積層体と接続されたそれぞれの負極外部端子がラミネートフィルム外装体の内部で重ねられており、前記重ねられた複数の正極外部端子および前記重ねられた複数の負極外部端子が、ラミネートフィルム外装体の同じ辺から外部に引き出されている請求項１に記載のラミネート形電池。   Each positive electrode external terminal connected to each positive electrode tab laminate is stacked inside the laminate film outer package, and each negative electrode external terminal connected to each negative electrode tab laminate is stacked inside the laminate film outer package. 2. The laminated battery according to claim 1, wherein the plurality of stacked positive electrode external terminals and the plurality of stacked negative electrode external terminals are drawn out from the same side of the laminate film exterior body. 集電体の少なくとも片面に正極合剤層を有するシート状正極と集電体の少なくとも片面に負極合剤層を有するシート状負極とがセパレータを介して積層されて渦巻き状に巻回された、横断面が略長円形の巻回電極体が、平面視で四角形のラミネートフィルム外装体に収容されており、前記ラミネートフィルム外装体の外周辺が熱シールされているラミネート形電池であって、
前記巻回電極体の巻回数が１０以上であり、
前記シート状正極の集電体の幅方向の端部は、正極合剤層が形成されずに正極タブとされ、
前記シート状負極の集電体の、前記正極タブとは反対側の幅方向の端部は、負極合剤層が形成されずに負極タブとされ、
前記シート状正極の正極タブは、前記巻回電極体の略長円形の平坦部において、複数の組に分けられて積層されることにより、複数の正極タブ積層体が形成されており、
前記シート状負極の負極タブは、前記巻回電極体の略長円形の平坦部において、複数の組に分けられて積層されることにより、複数の負極タブ積層体が形成されており、
前記正極タブ積層体は、それぞれ別の正極外部端子に接続され、かつ前記負極タブ積層体は、それぞれ別の負極外部端子に接続されており、
各正極外部端子および各負極外部端子同士は、それぞれラミネートフィルム外装体の内部または外部の少なくとも一方で互いに電気的に接続されていることを特徴とするラミネート形電池。 A sheet-like positive electrode having a positive electrode mixture layer on at least one side of the current collector and a sheet-like negative electrode having a negative electrode mixture layer on at least one side of the current collector were laminated via a separator and wound in a spiral shape, A spirally wound electrode body having a substantially oval cross section is housed in a rectangular laminate film exterior body in plan view, and is a laminate type battery in which the outer periphery of the laminate film exterior body is heat sealed,
The number of windings of the wound electrode body is 10 or more,
The widthwise end of the current collector of the sheet-like positive electrode is a positive electrode tab without forming a positive electrode mixture layer,
An end of the sheet-like negative electrode collector in the width direction opposite to the positive electrode tab is a negative electrode tab without forming a negative electrode mixture layer,
The positive electrode tab of the sheet-like positive electrode is divided into a plurality of sets and laminated in a substantially oval flat portion of the wound electrode body, thereby forming a plurality of positive electrode tab laminates,
The negative electrode tab of the sheet-like negative electrode is divided into a plurality of sets and laminated in a substantially oval flat part of the wound electrode body, thereby forming a plurality of negative electrode tab laminates,
Each of the positive electrode tab laminates is connected to another positive external terminal, and each of the negative electrode tab laminates is connected to another negative external terminal;
Each positive electrode external terminal and each negative electrode external terminal are electrically connected to each other at least either inside or outside of the laminate film outer package. 各正極タブ積層体と接続されたそれぞれの正極外部端子がラミネートフィルム外装体の内部で重ねられ、かつ各負極タブ積層体と接続されたそれぞれの負極外部端子がラミネートフィルム外装体の内部で重ねられており、前記重ねられた複数の正極外部端子および前記重ねられた複数の負極外部端子が、ラミネートフィルム外装体の対向する辺からそれぞれ外部に引き出されている請求項３に記載のラミネート形電池。   Each positive electrode external terminal connected to each positive electrode tab laminate is stacked inside the laminate film outer package, and each negative electrode external terminal connected to each negative electrode tab laminate is stacked inside the laminate film outer package. 4. The laminated battery according to claim 3, wherein the plurality of stacked positive electrode external terminals and the plurality of stacked negative electrode external terminals are respectively drawn out from opposite sides of the laminate film outer package. 複数の正極外部端子同士、および複数の負極外部端子同士が、ラミネートフィルム外装体の熱シール部において、ラミネートフィルム外装体の有する熱融着樹脂と同じ樹脂を含有する接着層を介して熱融着されている請求項１〜４のいずれかに記載のラミネート電池。   A plurality of positive external terminals and a plurality of negative external terminals are heat-sealed through an adhesive layer containing the same resin as the heat-seal resin of the laminate film exterior body in the heat seal portion of the laminate film exterior body. The laminated battery according to any one of claims 1 to 4.
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