JP2007273349A - Stacked battery and manufacturing method therefor - Google Patents

Stacked battery and manufacturing method therefor Download PDF

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JP2007273349A
JP2007273349A JP2006099091A JP2006099091A JP2007273349A JP 2007273349 A JP2007273349 A JP 2007273349A JP 2006099091 A JP2006099091 A JP 2006099091A JP 2006099091 A JP2006099091 A JP 2006099091A JP 2007273349 A JP2007273349 A JP 2007273349A
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active material
material layer
negative electrode
current collector
positive electrode
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Kenji Kimura
健治 木村
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Toyota Motor Corp
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Priority to PCT/JP2007/057021 priority patent/WO2007114311A1/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
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/04—Construction or manufacture in general
    • H01M10/0413—Large-sized flat cells or batteries for motive or stationary systems with plate-like electrodes
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—Construction or manufacture
    • H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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

Abstract

<P>PROBLEM TO BE SOLVED: To provide a stacked battery ensuring insulation between a positive pole and a negative pole, and to provide a manufacturing method for the stacked battery. <P>SOLUTION: The stacked battery includes a positive pole current-collecting foil 31 and a negative pole current-collecting foil 36 that are in a stacked arrangement, a positive pole active material layer 32 serving as a positive pole, a negative pole active material layer 37 serving as a negative pole, and an electrolytic layer 41, disposed in between the positive pole active material layer 32 and the negative pole active material layer 37. The negative pole current-collecting foil 36 has a surface 36a, and the positive pole current-collecting foil 31 has a surface 31a, and the surfaces 36a and 31a face each other. The negative pole active material layer 37 is formed on the surface 36a, and the positive pole active material layer 32 faces the negative pole active material layer 37 and is formed on the surface 31a. The ends 41u of the electrolytic layer 41 contact the surface 36a. The negative pole active material layer 37 is covered by the electrolytic layer 41. <P>COPYRIGHT: (C)2008,JPO&INPIT

Description

この発明は、一般的には、積層型電池およびその製造方法に関し、より特定的には、固体電解質を備える積層型電池およびその製造方法に関する。   The present invention generally relates to a stacked battery and a method for manufacturing the same, and more specifically to a stacked battery including a solid electrolyte and a method for manufacturing the same.

従来の積層型電池に関して、たとえば、特開２００４−１５８２２２号公報には、フォトレジスト工程を必要とせず、製造プロセスの大幅な簡略化が図られる多層積層電池が開示されている（特許文献１）。特許文献１に開示された多層積層電池は、正極および負極活物質層、この間に配置される固体電解質層、活物質層の直上、直下に配置される集電体層の５層からなる電池セルが複数段、重ね合わされて構成されている。電池セルを構成する各層は、その周縁部の幅が、活物質層、集電体層、固体電解質層の順に広くなるように形成されている。すなわち、固体電解質層が、活物質層の周縁および集電体の周縁を覆うように設けられている。   Regarding a conventional laminated battery, for example, Japanese Patent Application Laid-Open No. 2004-158222 discloses a multilayer laminated battery that does not require a photoresist process and greatly simplifies the manufacturing process (Patent Document 1). . The multilayer laminated battery disclosed in Patent Document 1 is a battery cell comprising five layers of a positive electrode and a negative electrode active material layer, a solid electrolyte layer disposed therebetween, and a current collector layer disposed immediately above and immediately below the active material layer. Are stacked in multiple stages. Each layer constituting the battery cell is formed so that the width of the peripheral portion thereof becomes wider in the order of the active material layer, the current collector layer, and the solid electrolyte layer. That is, the solid electrolyte layer is provided so as to cover the periphery of the active material layer and the periphery of the current collector.

また、特開２００４−３２７３７４号公報には、単電池層およびシール部材間に形成される隙間に起因して、短絡が発生することを防止するバイポーラ電池が開示されている（特許文献２）。特許文献２では、集電体の一方の面に正極活物層が形成され、他方の面に負極活物質層が形成されてなるバイポーラ電極が、ゲル状電解質を挟んで積層されている。正極活物質層、負極活物質層およびゲル状電解質の周囲には、絶縁性の粉末からなる絶縁部材が充填されている。
特開２００４−１５８２２２号公報 特開２００４−３２７３７４号公報 Japanese Patent Application Laid-Open No. 2004-327374 discloses a bipolar battery that prevents a short circuit from occurring due to a gap formed between a single battery layer and a seal member (Patent Document 2). In Patent Document 2, a bipolar electrode in which a positive electrode active material layer is formed on one surface of a current collector and a negative electrode active material layer is formed on the other surface is laminated with a gel electrolyte interposed therebetween. An insulating member made of an insulating powder is filled around the positive electrode active material layer, the negative electrode active material layer, and the gel electrolyte.
JP 2004-158222 A JP 2004-327374 A

上述の特許文献１では、正極および負極活物質層の方形状周辺を、電解質層および集電体層によって絶縁し、さらに集電体層の外縁部を固体電解質層によって絶縁している。しかしながら、電解質層および集電体層の双方の側部を包み込むように固体電解質層を設けた場合、多層積層電池の厚みが、固体電解質層の塑性変形の限度内に限られるという制約が生じる。   In the above-described Patent Document 1, the rectangular periphery of the positive electrode and the negative electrode active material layer is insulated by the electrolyte layer and the current collector layer, and the outer edge of the current collector layer is insulated by the solid electrolyte layer. However, when the solid electrolyte layer is provided so as to wrap both sides of the electrolyte layer and the current collector layer, there is a restriction that the thickness of the multilayer laminated battery is limited to the limit of plastic deformation of the solid electrolyte layer.

すなわち、特許文献１では、多層積層電池の最上段に配置される固体電解質層が、積層された活物質層および集電体の全体を包み込むように設けられる。このため、たとえば、電池セルの積層数が多くなったり、高容量を得る目的で活物質層の厚みが大きくなった場合には、固体電解質層に成形される曲げ形状が、固体電解質層の塑性変形の限度を越え、固体電解質層が破断するおそれが生じる。この場合、正極および負極活物資層間を適切に絶縁することができない。   That is, in Patent Document 1, the solid electrolyte layer disposed at the uppermost stage of the multilayer stacked battery is provided so as to enclose the entire stacked active material layer and current collector. For this reason, for example, when the number of battery cells is increased or the thickness of the active material layer is increased for the purpose of obtaining a high capacity, the bent shape formed in the solid electrolyte layer is the plasticity of the solid electrolyte layer. The deformation limit may be exceeded and the solid electrolyte layer may break. In this case, the positive electrode and negative electrode active material layers cannot be properly insulated.

そこでこの発明の目的は、上記の課題を解決することであり、正極および負極間の絶縁が確保される積層型電池およびその製造方法を提供することである。   Accordingly, an object of the present invention is to solve the above-described problems, and to provide a stacked battery in which insulation between a positive electrode and a negative electrode is ensured and a method for manufacturing the same.

この発明に従った積層型電池は、積層された第１および第２の集電体と、正極および負極のいずれか一方をなす第１の活物質層と、正極および負極のいずれか他方をなす第２の活物質層と、第１の活物質層と第２の活物質層との間に配置された固体電解質とを備える。第１の集電体は、第１の表面を有し、第２の集電体は、第２の表面を有する。第１の表面と第２の表面とは互いに向い合う。第１の活物質層は、第１の表面上に形成されている
。第２の活物質層は、第１の活物質層と対向し、第２の表面上に形成されている。固体電解質の端部は、第１の表面上に接触する。第１の活物質層は、固体電解質によって覆われている。 The stacked battery according to the present invention includes the stacked first and second current collectors, the first active material layer forming one of the positive electrode and the negative electrode, and the other of the positive electrode and the negative electrode. A second active material layer; and a solid electrolyte disposed between the first active material layer and the second active material layer. The first current collector has a first surface, and the second current collector has a second surface. The first surface and the second surface face each other. The first active material layer is formed on the first surface. The second active material layer faces the first active material layer and is formed on the second surface. The end of the solid electrolyte is in contact with the first surface. The first active material layer is covered with a solid electrolyte.

このように構成された積層型電池によれば、第１の活物質層を覆う固体電解質によって、第１の活物質層と第２の活物質層との短絡を防ぐことができる。この際、固体電解質の端部は、第１の表面上に接触するため、固体電解質は、第１の活物質層および第１の集電体のうち第１の活物質層のみを覆うように設けられる。このため、固体電解質に過大な曲げ形状が生じることを防止し、第１の活物質層が固体電解質によって覆われた形態をより確実に得ることができる。これにより、第１の活物質層および第２の活物質層間の絶縁を確保することができる。   According to the stacked battery configured as described above, a short circuit between the first active material layer and the second active material layer can be prevented by the solid electrolyte covering the first active material layer. At this time, since the end portion of the solid electrolyte is in contact with the first surface, the solid electrolyte covers only the first active material layer of the first active material layer and the first current collector. Provided. For this reason, it can prevent that an excessive bending shape arises in a solid electrolyte, and can obtain more reliably the form with which the 1st active material layer was covered with the solid electrolyte. Thereby, insulation between the first active material layer and the second active material layer can be ensured.

また好ましくは、第２の活物質層は、固体電解質によって覆われている。このように構成された積層型電池によれば、第１および第２の活物質層を固体電解質により覆うことによって、第１および第２の活物質層の一部が欠落することを防止できる。これにより、第１の活物質層と第２の活物質層との短絡を防ぐことに加えて、活物質層の欠落に起因した電池容量の低下を防ぐことができる。   Preferably, the second active material layer is covered with a solid electrolyte. According to the stacked battery configured as described above, it is possible to prevent the first and second active material layers from being partially lost by covering the first and second active material layers with the solid electrolyte. Thereby, in addition to preventing a short circuit between the first active material layer and the second active material layer, it is possible to prevent a decrease in battery capacity due to the lack of the active material layer.

この発明に従った積層型電池の製造方法は、上述のいずれかに記載の積層型電池の製造方法である。積層型電池の製造方法は、第１および第２の表面上に、それぞれ第１および第２の活物質層を形成する工程と、第１の活物質層を覆うように、第１の表面上に固体電解質を形成する工程と、固体電解質を形成する工程の後、第１の集電体と第２の集電体とを積層する工程とを備える。   A method for manufacturing a stacked battery according to the present invention is the method for manufacturing a stacked battery according to any one of the above. The method for manufacturing a stacked battery includes a step of forming first and second active material layers on the first and second surfaces, respectively, and the first surface so as to cover the first active material layer. And a step of laminating a first current collector and a second current collector after the step of forming the solid electrolyte and the step of forming the solid electrolyte.

このように構成された積層型電池の製造方法によれば、第１の集電体と第２の集電体とを積層する前に、予め第１の活物質層を固体電解質により覆うことによって、第１の活物質層と第２の活物質層との短絡を確実に防止できる。   According to the method for manufacturing a stacked battery configured as described above, the first active material layer is covered with a solid electrolyte in advance before the first current collector and the second current collector are stacked. It is possible to reliably prevent a short circuit between the first active material layer and the second active material layer.

以上説明したように、この発明に従えば、正極および負極間の絶縁が確保される積層型電池およびその製造方法を提供することができる。   As described above, according to the present invention, it is possible to provide a stacked battery in which insulation between the positive electrode and the negative electrode is ensured and a method for manufacturing the same.

この発明の実施の形態について、図面を参照して説明する。なお、以下で参照する図面では、同一またはそれに相当する部材には、同じ番号が付されている。   Embodiments of the present invention will be described with reference to the drawings. In the drawings referred to below, the same or corresponding members are denoted by the same reference numerals.

（実施の形態１）
図１は、この発明の実施の形態１における積層型電池を示す断面図である。図１を参照して、積層型電池１０は、ガソリンエンジンやディーゼルエンジン等の内燃機関と、充放電可能な電源とを動力源とするハイブリッド自動車に電源として搭載される。積層型電池１０は、リチウムイオン電池から形成されている。 (Embodiment 1)
1 is a cross-sectional view showing a stacked battery according to Embodiment 1 of the present invention. Referring to FIG. 1, stacked battery 10 is mounted as a power source in a hybrid vehicle that uses an internal combustion engine such as a gasoline engine or a diesel engine and a power source that can be charged and discharged as a power source. The stacked battery 10 is formed from a lithium ion battery.

積層型電池１０は、矢印１０１に示す方向に積層された複数の単電池３０を備える。積層型電池１０は、略直方体形状を有する。積層型電池１０は、単電池３０の積層方向の長さが他の辺の長さよりも小さい薄板形状を有しても良い。複数の単電池３０は、電気的に直列に接続されている。積層型電池１０は、たとえば、２００Ｖ以上の電圧を有する。積層型電池１０は、たとえば５０以上の単電池３０を備える。   The stacked battery 10 includes a plurality of single cells 30 stacked in the direction indicated by the arrow 101. The stacked battery 10 has a substantially rectangular parallelepiped shape. The stacked battery 10 may have a thin plate shape in which the length of the unit cells 30 in the stacking direction is smaller than the length of the other side. The plurality of unit cells 30 are electrically connected in series. The stacked battery 10 has a voltage of 200 V or more, for example. The stacked battery 10 includes, for example, 50 or more unit cells 30.

各単電池３０は、シート状の正極集電箔３１および負極集電箔３６を有する。複数の単電池３０は、互いに隣り合う単電池３０間で、正極集電箔３１と負極集電箔３６とが隣接
するように積層されている。単電池３０の積層方向の一方端に配置された正極集電箔３１には、正極端子２６が接続されている。単電池３０の積層方向の他方端に配置された負極集電箔３６には、負極端子２７が接続されている。 Each unit cell 30 has a sheet-like positive electrode current collector foil 31 and a negative electrode current collector foil 36. The plurality of single cells 30 are stacked such that the positive electrode current collector foil 31 and the negative electrode current collector foil 36 are adjacent to each other between the adjacent single cells 30. A positive electrode terminal 26 is connected to the positive electrode current collector foil 31 disposed at one end in the stacking direction of the unit cells 30. A negative electrode terminal 27 is connected to the negative electrode current collector foil 36 disposed at the other end in the stacking direction of the unit cells 30.

積層された複数の単電池３０は、外装体としてのラミネートフィルム２８によって覆われている。ラミネートフィルム２８としては、たとえば、アルミニウムからなる基材にポリエチレンテレフタラート樹脂（ＰＥＴ：poly ethylene terephthalate）が被膜されたものが使用される。ラミネートフィルム２８は、主に水分の浸入を防止するために設けられている。単電池３０が有する電解質の種類によっては、ラミネートフィルム２８が省略されることもある。   The plurality of unit cells 30 stacked are covered with a laminate film 28 as an exterior body. As the laminate film 28, for example, a film in which a polyethylene terephthalate (PET) film is coated on a base material made of aluminum is used. The laminate film 28 is provided mainly to prevent moisture from entering. Depending on the type of electrolyte that the unit cell 30 has, the laminate film 28 may be omitted.

積層された複数の単電池３０の両側には、拘束板２１および２３が配設されている。拘束板２１と拘束板２３とは、単電池３０の積層方向に延びるボルト２４によって互いに結合されている。ボルト２４の軸力によって、複数の単電池３０はその積層方向に拘束されている。なお、本実施の形態では、複数の単電池３０を拘束する拘束部材として、ボルト２４を用いたが、これに限定されず、たとえば単電池３０の積層方向に締め付け力を発生させるゴムや紐、バンド、テープ等であっても良い。   Restraint plates 21 and 23 are disposed on both sides of the plurality of stacked unit cells 30. The restraint plate 21 and the restraint plate 23 are coupled to each other by a bolt 24 extending in the stacking direction of the unit cells 30. The plurality of unit cells 30 are restrained in the stacking direction by the axial force of the bolts 24. In the present embodiment, the bolt 24 is used as a restraining member that restrains the plurality of single cells 30, but is not limited to this, for example, a rubber or string that generates a tightening force in the stacking direction of the single cells 30, A band, a tape, etc. may be sufficient.

互いに隣り合う複数の単電池３０間には、正極集電箔３１と負極集電箔３６とに挟持されるようにシート部材４６が配設されている。シート部材４６は、正極集電箔３１と負極集電箔３６との間から延出する冷却用タブ４７を有する。冷却用タブ４７は、ラミネートフィルム２８の外側に引き出されている。シート部材４６は、熱伝導性に優れた導電性材料から形成されている。シート部材４６は、たとえば、アルミニウム、銅もしくはカーボンシートから形成されている。このような構成により、単電池３０で発生した熱は、シート部材４６の冷却用タブ４７に伝わって、ラミネートフィルム２８の外側に効率良く放熱される。なお、シート部材４６は、必ずしも設けられる必要はない。   A sheet member 46 is disposed between the plurality of unit cells 30 adjacent to each other so as to be sandwiched between the positive electrode current collector foil 31 and the negative electrode current collector foil 36. The sheet member 46 has a cooling tab 47 extending from between the positive electrode current collector foil 31 and the negative electrode current collector foil 36. The cooling tab 47 is drawn out of the laminate film 28. The sheet member 46 is formed from a conductive material having excellent thermal conductivity. The sheet member 46 is made of, for example, aluminum, copper, or a carbon sheet. With such a configuration, the heat generated in the unit cell 30 is transmitted to the cooling tab 47 of the sheet member 46 and efficiently dissipated to the outside of the laminate film 28. Note that the sheet member 46 is not necessarily provided.

図２は、図１中の積層型電池が備える単電池を示す断面図である。図２を参照して、単電池３０は、正極集電箔３１および負極集電箔３６に加えて、正極集電箔３１および負極集電箔３６にそれぞれ設けられた正極活物質層３２および負極活物質層３７と、正極活物質層３２と負極活物質層３７との間に設けられた電解質層４１とを有する。本実施の形態における積層型電池１０は、正極活物質層３２および負極活物質層３７が２枚の集電箔に別々に設けられる２次電池である。   FIG. 2 is a cross-sectional view showing a unit cell included in the stacked battery in FIG. Referring to FIG. 2, in addition to positive electrode current collector foil 31 and negative electrode current collector foil 36, unit cell 30 includes positive electrode active material layer 32 and negative electrode provided on positive electrode current collector foil 31 and negative electrode current collector foil 36, respectively. An active material layer 37 and an electrolyte layer 41 provided between the positive electrode active material layer 32 and the negative electrode active material layer 37 are included. The laminated battery 10 in the present embodiment is a secondary battery in which the positive electrode active material layer 32 and the negative electrode active material layer 37 are separately provided on two current collector foils.

正極集電箔３１および負極集電箔３６は、表面３１ａおよび表面３６ａをそれぞれ有する。正極集電箔３１および負極集電箔３６は、表面３１ａと表面３６ａとが互いに距離を隔てて向い合うように、矢印１０１に示す単電池３０の積層方向に重ね合わされている。表面３１ａと表面３６ａとは、単電池３０の積層方向に直交する平面内で互いに平行に延在している。   The positive electrode current collector foil 31 and the negative electrode current collector foil 36 have a surface 31a and a surface 36a, respectively. The positive electrode current collector foil 31 and the negative electrode current collector foil 36 are overlapped in the stacking direction of the unit cells 30 indicated by the arrow 101 so that the surface 31a and the surface 36a face each other with a distance therebetween. The surface 31a and the surface 36a extend parallel to each other in a plane orthogonal to the stacking direction of the unit cells 30.

複数の単電池３０が有する正極集電箔３１は、全て同一形状に形成されている。複数の単電池３０が有する負極集電箔３６は、全て同一形状に形成されている。正極集電箔３１は、たとえばアルミニウムから形成されている。負極集電箔３６は、たとえば銅から形成されている。   The positive electrode current collector foils 31 included in the plurality of single cells 30 are all formed in the same shape. The negative electrode current collector foils 36 included in the plurality of single cells 30 are all formed in the same shape. The positive electrode current collector foil 31 is made of, for example, aluminum. The negative electrode current collector foil 36 is made of, for example, copper.

正極活物質層３２および負極活物質層３７は、表面３１ａおよび表面３６ａ上にそれぞれ形成されている。正極活物質層３２は、正極集電箔３１の表面上であって、負極集電箔３６側に形成されている。負極活物質層３７は、負極集電箔３６の表面上であって、正極集電箔３１側に形成されている。正極活物質層３２と負極活物質層３７とは、電解質層４１を介して互いに対向する。   The positive electrode active material layer 32 and the negative electrode active material layer 37 are formed on the surface 31a and the surface 36a, respectively. The positive electrode active material layer 32 is formed on the surface of the positive electrode current collector foil 31 and on the negative electrode current collector foil 36 side. The negative electrode active material layer 37 is formed on the surface of the negative electrode current collector foil 36 and on the positive electrode current collector foil 31 side. The positive electrode active material layer 32 and the negative electrode active material layer 37 face each other with the electrolyte layer 41 interposed therebetween.

電解質層４１は、イオン伝導性を示す材料から形成される層である。電解質層４１を介在させることによって、正極活物質層３２および負極活物質層３７間のイオン伝導がスムーズになり、積層型電池１０の出力を向上させることができる。電解質層４１は、固体電解質から形成されている。   The electrolyte layer 41 is a layer formed from a material exhibiting ionic conductivity. By interposing the electrolyte layer 41, ion conduction between the positive electrode active material layer 32 and the negative electrode active material layer 37 becomes smooth, and the output of the stacked battery 10 can be improved. The electrolyte layer 41 is formed from a solid electrolyte.

単電池３０は、絶縁材料から形成された絶縁部材としての絶縁樹脂４５をさらに有する。絶縁樹脂４５は、正極集電箔３１と負極集電箔３６との間で表面３１ａおよび３６ａの周縁に沿って設けられている。絶縁樹脂４５は、正極活物質層３２、負極活物質層３７および電解質層４１の周囲を取り囲むように設けられている。絶縁樹脂４５は、電解質層４１に接触して設けられている。正極活物質層３２、負極活物質層３７および電解質層４１は、絶縁樹脂４５によって、正極集電箔３１と負極集電箔３６との間の空間に封入されている。絶縁樹脂４５は、絶縁材料から形成されており、たとえばエポキシ樹脂、アクリル樹脂、シリコーンゴムもしくはフッ素ゴムから形成されている。   The unit cell 30 further includes an insulating resin 45 as an insulating member formed from an insulating material. The insulating resin 45 is provided along the peripheral edges of the surfaces 31 a and 36 a between the positive electrode current collector foil 31 and the negative electrode current collector foil 36. The insulating resin 45 is provided so as to surround the periphery of the positive electrode active material layer 32, the negative electrode active material layer 37, and the electrolyte layer 41. The insulating resin 45 is provided in contact with the electrolyte layer 41. The positive electrode active material layer 32, the negative electrode active material layer 37, and the electrolyte layer 41 are enclosed in a space between the positive electrode current collector foil 31 and the negative electrode current collector foil 36 by an insulating resin 45. The insulating resin 45 is made of an insulating material, and is made of, for example, an epoxy resin, an acrylic resin, silicone rubber, or fluorine rubber.

正極活物質層３２は、負極活物質層３７に対向する頂面３２ａと、頂面３２ａから表面３１ａに連なる側面３２ｂとを有する。負極活物質層３７は、正極活物質層３２に対向する頂面３７ａと、頂面３７ａから表面３６ａに連なる側面３７ｂとを有する。頂面３７ａおよび側面３７ｂは、表面３６ａから露出する負極活物質層３７の外表面を構成している。   The positive electrode active material layer 32 has a top surface 32a that faces the negative electrode active material layer 37, and a side surface 32b that extends from the top surface 32a to the surface 31a. The negative electrode active material layer 37 has a top surface 37a that faces the positive electrode active material layer 32, and a side surface 37b that extends from the top surface 37a to the surface 36a. The top surface 37a and the side surface 37b constitute the outer surface of the negative electrode active material layer 37 exposed from the surface 36a.

正極集電箔３１および負極集電箔３６は、単電池３０の積層方向に延在する側面３１ｂおよび３６ｂをそれぞれ有する。絶縁樹脂４５は、側面３１ｂおよび３６ｂと同一平面上に延在する側面４５ｂを有する。側面３１ｂおよび３６ｂと側面４５ｂとは、単電池３０の外殻をなす。このような構成により、絶縁樹脂４５によって、正極集電箔３１および負極集電箔３６の周縁部分が互いに離間した位置に確実に保持される。これにより、正極集電箔３１と負極集電箔３６とが、接触し、正極および負極間が短絡することを防止できる。また、絶縁樹脂４５によって、単電池３０の周縁が単電池３０の積層方向に沿って補強されることになるため、積層型電池１０の剛性を向上させることができる。   The positive electrode current collector foil 31 and the negative electrode current collector foil 36 have side surfaces 31 b and 36 b extending in the stacking direction of the unit cells 30, respectively. Insulating resin 45 has side surface 45b extending on the same plane as side surfaces 31b and 36b. The side surfaces 31 b and 36 b and the side surface 45 b form an outer shell of the unit cell 30. With such a configuration, the peripheral portions of the positive electrode current collector foil 31 and the negative electrode current collector foil 36 are reliably held at positions separated from each other by the insulating resin 45. Thereby, it can prevent that the positive electrode current collection foil 31 and the negative electrode current collection foil 36 contact, and short-circuit between a positive electrode and a negative electrode. In addition, since the peripheral edge of the unit cell 30 is reinforced along the stacking direction of the unit cells 30 by the insulating resin 45, the rigidity of the unit cell 10 can be improved.

図３は、図２中の単電池を構成する負極を示す斜視図である。図２および図３を参照して、電解質層４１は、負極活物質層３７を覆うように表面３６ａ上に設けられている。電解質層４１は、頂面３７ａおよび側面３７ｂの全体を覆うように設けられている。電解質層４１は、外表面４１ａを有する。外表面４１ａは、表面３６ａに連なっている。本実施の形態では、正極活物質層３２が電解質層４１によって覆われていない。電解質層４１は、頂面３２ａに接触するように設けられている。電解質層４１は、側面３２ｂと非接触となるように設けられている。   FIG. 3 is a perspective view showing a negative electrode constituting the unit cell in FIG. 2 and 3, electrolyte layer 41 is provided on surface 36 a so as to cover negative electrode active material layer 37. The electrolyte layer 41 is provided so as to cover the entire top surface 37a and side surface 37b. The electrolyte layer 41 has an outer surface 41a. The outer surface 41a is continuous with the surface 36a. In the present embodiment, the positive electrode active material layer 32 is not covered with the electrolyte layer 41. The electrolyte layer 41 is provided in contact with the top surface 32a. The electrolyte layer 41 is provided so as not to contact the side surface 32b.

電解質層４１は、端部４１ｕを有する。端部４１ｕは、電解質層４１の中で、単電池３０の積層方向に直交する平面内において最も周縁に配設される部分である。端部４１ｕは、表面３６ａ上に接触する。   The electrolyte layer 41 has an end 41u. The end portion 41u is a portion of the electrolyte layer 41 that is disposed at the most peripheral edge in a plane orthogonal to the stacking direction of the unit cells 30. The end 41u contacts the surface 36a.

単電池３０の積層方向、すなわち、正極集電箔３１および負極集電箔３６が重ね合わされた方向から見て、負極集電箔３６は、領域２００に形成され、電解質層４１は、領域３００に形成され、負極活物質層３７は、領域４００に形成されている。領域３００は、領域２００に含まれている。領域４００は、領域３００に含まれている。本実施の形態では、正極集電箔３１および負極集電箔３６が重ね合わされた方向から見て、領域２００、３００および４００が略矩形形状を有する。領域３００の縦横巾は、領域２００の縦横巾よりも小さい。領域４００の縦横幅は、領域３００の縦横巾よりも小さい。領域３００の面積は、領域２００の面積よりも小さい。領域４００の面積は、領域３００の面積よりも小
さい。 When viewed from the stacking direction of the unit cells 30, that is, the direction in which the positive electrode current collector foil 31 and the negative electrode current collector foil 36 are overlapped, the negative electrode current collector foil 36 is formed in the region 200, and the electrolyte layer 41 is formed in the region 300. The negative electrode active material layer 37 thus formed is formed in the region 400. The area 300 is included in the area 200. The area 400 is included in the area 300. In the present embodiment, the regions 200, 300, and 400 have a substantially rectangular shape when viewed from the direction in which the positive electrode current collector foil 31 and the negative electrode current collector foil 36 are overlapped. The vertical and horizontal width of the region 300 is smaller than the vertical and horizontal width of the region 200. The vertical and horizontal width of the region 400 is smaller than the vertical and horizontal width of the region 300. The area of the region 300 is smaller than the area of the region 200. The area of the region 400 is smaller than the area of the region 300.

このような構成により、電解質層４１は、負極集電箔３６および負極活物質層３７のうち負極活物質層３７のみを包み込むように設けられている。負極集電箔３６の側面３６ｂは、電解質層４１から露出している。   With such a configuration, the electrolyte layer 41 is provided so as to wrap only the negative electrode active material layer 37 among the negative electrode current collector foil 36 and the negative electrode active material layer 37. The side surface 36 b of the negative electrode current collector foil 36 is exposed from the electrolyte layer 41.

続いて、図２中の単電池３０を構成する各部材について詳細な説明を行なう。正極活物質層３２は、正極活物質および固体高分子電解質を含む。正極活物質層３２は、イオン伝導性を高めるための支持塩（リチウム塩）、電子伝導性を高めるための導電助剤、スラリー粘度の調整溶媒としてのＮＭＰ（Ｎ−メチル−２−ピロリドン）、重合開始剤としてのＡＩＢＮ（アゾビスイソブチロニトリル）等を含んでも良い。   Subsequently, each member constituting the single cell 30 in FIG. 2 will be described in detail. The positive electrode active material layer 32 includes a positive electrode active material and a solid polymer electrolyte. The positive electrode active material layer 32 includes a supporting salt (lithium salt) for increasing ionic conductivity, a conductive auxiliary agent for increasing electronic conductivity, NMP (N-methyl-2-pyrrolidone) as a solvent for adjusting slurry viscosity, AIBN (azobisisobutyronitrile) as a polymerization initiator may be included.

正極活物質としては、リチウムイオン２次電池で一般的に用いられる、リチウムと遷移金属との複合酸化物を使用することができる。正極活物質として、たとえば、ＬｉＣｏＯ２等のＬｉ・Ｃｏ系複合酸化物、ＬｉＮｉＯ２等のＬｉ・Ｎｉ系複合酸化物、スピネルＬｉＭｎ２Ｏ４等のＬｉ・Ｍｎ系複合酸化物、ＬｉＦｅＯ２等のＬｉ・Ｆｅ系複合酸化物などが挙げられる。その他、ＬｉＦｅＰＯ４等の遷移金属とリチウムとのリン酸化合物や硫酸化合物；Ｖ２Ｏ５、ＭｎＯ２、ＴｉＳ２、ＭｏＳ２、ＭｏＯ３等の遷移金属酸化物や硫化物；ＰｂＯ２、ＡｇＯ、ＮｉＯＯＨ等が挙げられる。 As the positive electrode active material, a composite oxide of lithium and a transition metal, which is generally used in a lithium ion secondary battery, can be used. As the positive electrode active material, for example, Li · Co-based composite oxide such as LiCoO 2, Li · Ni-based composite oxide such as LiNiO 2, Li · Mn-based composite oxide such as spinel LiMn 2 O 4, such as LiFeO 2 Examples include Li · Fe-based composite oxides. In addition, transition metal oxides such as LiFePO 4 and lithium and sulfuric acid compounds; transition metal oxides and sulfides such as V 2 O 5 , MnO 2 , TiS 2 , MoS 2 , MoO 3 ; PbO 2 , AgO, NiOOH etc. are mentioned.

固体高分子電解質は、イオン伝導性を示す高分子であれば、特に限定されず、たとえば、ポリエチレンオキシド（ＰＥＯ）、ポリプロピレンオキシド（ＰＰＯ）、これらの共重合体などが挙げられる。このようなポリアルキレンオキシド系高分子は、ＬｉＢＦ４、ＬｉＰＦ６、ＬｉＮ（ＳＯ２ＣＦ３）２、ＬｉＮ（ＳＯ２Ｃ２Ｆ５）２等のリチウム塩を容易に溶解する。固体高分子電解質は、正極活物質層３２および負極活物質層３７の少なくとも一方に含まれる。より好ましくは、固体高分子電解質は、正極活物質層３２および負極活物質層３７の双方に含まれる。 The solid polymer electrolyte is not particularly limited as long as it is a polymer exhibiting ion conductivity, and examples thereof include polyethylene oxide (PEO), polypropylene oxide (PPO), and copolymers thereof. Such a polyalkylene oxide polymer readily dissolves lithium salts such as LiBF 4 , LiPF 6 , LiN (SO 2 CF 3 ) 2 , and LiN (SO 2 C 2 F 5 ) 2 . The solid polymer electrolyte is contained in at least one of the positive electrode active material layer 32 and the negative electrode active material layer 37. More preferably, the solid polymer electrolyte is included in both the positive electrode active material layer 32 and the negative electrode active material layer 37.

支持塩としては、Ｌｉ（Ｃ２Ｆ５ＳＯ２）２Ｎ、ＬｉＢＦ４、ＬｉＰＦ６、ＬｉＮ（ＳＯ２Ｃ２Ｆ５）２、もしくはこれらの混合物等を使用することができる。導電助剤としては、アセチレンブラック、カーボンブラック、グラファイト等を使用することができる。 As the supporting salt, Li (C 2 F 5 SO 2 ) 2 N, LiBF 4 , LiPF 6 , LiN (SO 2 C 2 F 5 ) 2 , or a mixture thereof can be used. As the conductive auxiliary agent, acetylene black, carbon black, graphite or the like can be used.

負極活物質層３７は、負極活物質および固体高分子電解質を含む。負極活物質層は、イオン伝導性を高めるための支持塩（リチウム塩）、電子伝導性を高めるための導電助剤、スラリー粘度の調整溶媒としてのＮＭＰ（Ｎ−メチル−２−ピロリドン）、重合開始剤としてのＡＩＢＮ（アゾビスイソブチロニトリル）等を含んでも良い。   The negative electrode active material layer 37 includes a negative electrode active material and a solid polymer electrolyte. The negative electrode active material layer is composed of a supporting salt (lithium salt) for increasing ion conductivity, a conductive auxiliary agent for increasing electronic conductivity, NMP (N-methyl-2-pyrrolidone) as a solvent for adjusting slurry viscosity, polymerization AIBN (azobisisobutyronitrile) as an initiator may be included.

負極活物質としては、リチウムイオン２次電池で一般的に用いられる材料を使用することができる。但し、固体電解質を使用する場合、負極活物質として、カーボンもしくはリチウムと金属酸化物もしくは金属との複合酸化物を用いることが好ましい。より好ましくは、負極活物質は、カーボンもしくはリチウムと遷移金属との複合酸化物である。さらに好ましくは、遷移金属はチタンである。つまり、負極活物質は、チタン酸化物もしくはチタンとリチウムとの複合酸化物であることがさらに好ましい。   As a negative electrode active material, the material generally used with a lithium ion secondary battery can be used. However, when a solid electrolyte is used, it is preferable to use a composite oxide of carbon or lithium and a metal oxide or metal as the negative electrode active material. More preferably, the negative electrode active material is a composite oxide of carbon or lithium and a transition metal. More preferably, the transition metal is titanium. That is, the negative electrode active material is more preferably titanium oxide or a composite oxide of titanium and lithium.

電解質層４１を形成する固体電解質としては、たとえば、ポリエチレンオキシド（ＰＥＯ）、ポリプロピレンオキシド（ＰＰＯ）、これらの共重合体等、固体高分子電解質を使用することができる。固体電解質は、イオン伝導性を確保するための支持塩（リチウム塩）を含む。支持塩としては、ＬｉＢＦ４、ＬｉＰＦ６、ＬｉＮ（ＳＯ２ＣＦ３）２、ＬｉＮ（ＳＯ２Ｃ２Ｆ５）２、もしくはこれらの混合物等を使用することができる。 As the solid electrolyte forming the electrolyte layer 41, for example, a solid polymer electrolyte such as polyethylene oxide (PEO), polypropylene oxide (PPO), or a copolymer thereof can be used. The solid electrolyte includes a supporting salt (lithium salt) for ensuring ionic conductivity. As the supporting salt, LiBF 4 , LiPF 6 , LiN (SO 2 CF 3 ) 2 , LiN (SO 2 C 2 F 5 ) 2 , or a mixture thereof can be used.

さらに、正極活物質層３２、負極活物質層３７および電解質層４１を形成する材料の具体例を表１および表２に示す。表１は、電解質層４１が有機系固体電解質である場合の具体例であり、表２は、電解質層４１が無機系固体電解質である場合の具体例である。   Further, specific examples of materials for forming the positive electrode active material layer 32, the negative electrode active material layer 37, and the electrolyte layer 41 are shown in Tables 1 and 2. Table 1 is a specific example when the electrolyte layer 41 is an organic solid electrolyte, and Table 2 is a specific example when the electrolyte layer 41 is an inorganic solid electrolyte.

Figure 2007273349
Figure 2007273349

Figure 2007273349
Figure 2007273349

続いて、図２中の単電池３０の製造方法について説明を行なう。図４から図９は、図２中の単電池の製造方法の工程を示す断面図である。図４を参照して、スパッタリング等の成膜工程により、正極集電箔３１の表面３１ａ上に正極活物質層３２を形成する。図５を参照して、正極活物質層３２の周囲を取り囲むように、表面３１ａ上に絶縁樹脂４５を塗布する。   Then, the manufacturing method of the cell 30 in FIG. 2 is demonstrated. 4 to 9 are cross-sectional views showing the steps of the method for manufacturing the unit cell in FIG. Referring to FIG. 4, positive electrode active material layer 32 is formed on surface 31 a of positive electrode current collector foil 31 by a film formation process such as sputtering. Referring to FIG. 5, insulating resin 45 is applied on surface 31 a so as to surround the periphery of positive electrode active material layer 32.

図６を参照して、図４に示す工程と同様に、負極集電箔３６の表面３６ａ上に負極活物質層３７を形成する。さらに、その負極活物質層３７を覆うように表面３６ａ上に電解質層４１を形成する。図７を参照して、負極活物質層３７および電解質層４１の周囲を取り囲むように、表面３６ａ上に絶縁樹脂４５を塗布する。なお、図４および図５中に示す正極形成工程と、図６および図７中に示す負極形成工程とは、同時に行なっても良いし、前後して行なっても良い。   Referring to FIG. 6, a negative electrode active material layer 37 is formed on the surface 36 a of the negative electrode current collector foil 36 in the same manner as the process shown in FIG. 4. Further, an electrolyte layer 41 is formed on the surface 36 a so as to cover the negative electrode active material layer 37. Referring to FIG. 7, insulating resin 45 is applied on surface 36 a so as to surround the periphery of negative electrode active material layer 37 and electrolyte layer 41. Note that the positive electrode forming step shown in FIGS. 4 and 5 and the negative electrode forming step shown in FIGS. 6 and 7 may be performed simultaneously or before and after.

図８を参照して、正極集電箔３１と負極集電箔３６とを互いに重ね合わせる。正極集電箔３１および負極集電箔３６にそれぞれ塗布した絶縁樹脂４５を、互いに接触した状態で硬化させる。これにより、正極集電箔３１と負極集電箔３６とが一体化される。図９を参照して、正極集電箔３１および負極集電箔３６の周縁を切断する。このとき、切断面として、正極集電箔３１の側面３１ｂ、負極集電箔３６の側面３６ｂおよび絶縁樹脂４５の側面４５ｂが形成される。以上の工程により、図２中の単電池３０が完成する。   Referring to FIG. 8, positive electrode current collector foil 31 and negative electrode current collector foil 36 are overlapped with each other. The insulating resin 45 applied to each of the positive electrode current collector foil 31 and the negative electrode current collector foil 36 is cured while being in contact with each other. Thereby, the positive electrode current collector foil 31 and the negative electrode current collector foil 36 are integrated. Referring to FIG. 9, the periphery of positive electrode current collector foil 31 and negative electrode current collector foil 36 is cut. At this time, the side surface 31b of the positive electrode current collector foil 31, the side surface 36b of the negative electrode current collector foil 36, and the side surface 45b of the insulating resin 45 are formed as cut surfaces. The unit cell 30 in FIG. 2 is completed through the above steps.

図１０は、図４および図５中に示す工程を経て得られた正極集電箔を示す斜視図である。図１０を参照して、図４および図５中に示す工程において、１枚の正極集電箔１３１上の間隔を隔てた複数箇所に、それぞれ正極活物質層３２および絶縁樹脂４５を形成しても良い。同様に、図６および図７中に示す工程において、１枚の負極集電箔上の間隔を隔てた複数箇所に、それぞれ負極活物質層３７、電解質層４１および絶縁樹脂４５を形成しても良い。その後、図８および図９中にそれぞれ示す積層工程および切断工程を実施することによって、複数の単電池３０を一括に作製することができる。   FIG. 10 is a perspective view showing a positive electrode current collector foil obtained through the steps shown in FIGS. 4 and 5. Referring to FIG. 10, in the steps shown in FIGS. 4 and 5, positive electrode active material layer 32 and insulating resin 45 are respectively formed at a plurality of positions on one positive electrode current collector foil 131 at intervals. Also good. Similarly, in the steps shown in FIGS. 6 and 7, the negative electrode active material layer 37, the electrolyte layer 41, and the insulating resin 45 may be formed at a plurality of positions on the single negative electrode current collector foil at intervals. good. Thereafter, a plurality of unit cells 30 can be manufactured in a lump by performing the stacking step and the cutting step shown in FIGS. 8 and 9, respectively.

この発明の実施の形態１における積層型電池１０は、積層された第１および第２の集電体としての負極集電箔３６および正極集電箔３１と、正極および負極のいずれか一方としての負極をなす第１の活物質層としての負極活物質層３７と、正極および負極のいずれか他方としての正極をなす第２の活物質層としての正極活物質層３２と、負極活物質層３７と正極活物質層３２との間に配置された固体電解質としての電解質層４１とを備える。負極集電箔３６は、第１の表面としての表面３６ａを有し、正極集電箔３１は、第２の表面としての表面３１ａを有する。表面３６ａと表面３１ａとは互いに向い合う。負極活物質層３７は、表面３６ａ上に形成されている。正極活物質層３２は、負極活物質層３７と対向し、表面３１ａ上に形成されている。電解質層４１の端部４１ｕは、表面３６ａ上に接触する。負極活物質層３７は、電解質層４１によって覆われている。   A laminated battery 10 according to Embodiment 1 of the present invention includes a negative electrode current collector foil 36 and a positive electrode current collector foil 31 as stacked first and second current collectors, and one of a positive electrode and a negative electrode. A negative electrode active material layer 37 as a first active material layer forming a negative electrode, a positive electrode active material layer 32 as a second active material layer forming a positive electrode as either the positive electrode or the negative electrode, and a negative electrode active material layer 37 And an electrolyte layer 41 as a solid electrolyte disposed between the positive electrode active material layer 32. The negative electrode current collector foil 36 has a surface 36a as a first surface, and the positive electrode current collector foil 31 has a surface 31a as a second surface. The surface 36a and the surface 31a face each other. The negative electrode active material layer 37 is formed on the surface 36a. The positive electrode active material layer 32 faces the negative electrode active material layer 37 and is formed on the surface 31a. The end 41u of the electrolyte layer 41 is in contact with the surface 36a. The negative electrode active material layer 37 is covered with an electrolyte layer 41.

この発明の実施の形態１における積層型電池１０は、積層された第１および第２の集電体としての負極集電箔３６および正極集電箔３１と、負極集電箔３６の表面３６ａ上に形成され、正極および負極のいずれか一方としての負極をなす第１の活物質層としての負極活物質層３７と、正極集電箔３１の表面３１ａ上に形成され、負極活物質層３７と対向し、正極および負極のいずれか他方としての正極をなす第２の活物質層としての正極活物質層３２と、負極活物質層３７と正極活物質層３２との間に配置された固体電解質としての電解質層４１とを備える。負極集電箔３６および正極集電箔３１の積層方向から見て、負極集電箔３６は、第１の領域としての領域２００に設けられ、電解質層４１は、第２の領域としての領域３００に設けられ、負極活物質層３７は、第３の領域としての領域４００に設けられている。この場合に、領域３００は、領域２００に含まれ、領域４００は、領域３００に含まれている。負極活物質層３７は、電解質層４１によって覆われている。   A laminated battery 10 according to Embodiment 1 of the present invention includes a negative electrode current collector foil 36 and a positive electrode current collector foil 31 as first and second current collectors stacked, and a surface 36 a of the negative electrode current collector foil 36. A negative electrode active material layer 37 as a first active material layer that forms a negative electrode as one of a positive electrode and a negative electrode, and a negative electrode active material layer 37 formed on the surface 31a of the positive electrode current collector foil 31. A positive electrode active material layer 32 as a second active material layer facing each other and forming a positive electrode as the other of the positive electrode and the negative electrode, and a solid electrolyte disposed between the negative electrode active material layer 37 and the positive electrode active material layer 32 As an electrolyte layer 41. When viewed from the stacking direction of the negative electrode current collector foil 36 and the positive electrode current collector foil 31, the negative electrode current collector foil 36 is provided in the region 200 as the first region, and the electrolyte layer 41 is the region 300 as the second region. The negative electrode active material layer 37 is provided in a region 400 as a third region. In this case, the region 300 is included in the region 200, and the region 400 is included in the region 300. The negative electrode active material layer 37 is covered with an electrolyte layer 41.

このように構成された積層型電池１０によれば、負極活物質層３７を電解質層４１で覆うことによって、正極活物質層３２が欠落することがあっても、その欠落した部分を介して正極活物質層３２と負極活物質層３７とが短絡することを防止できる。また、電解質層４１は、負極活物質層３７および負極集電箔３６のうちの負極活物質層３７のみを覆うように設けられるため、電解質層４１に過大な曲げ形状が生じることを抑制できる。これにより、電解質層４１の破断を防止し、正極活物質層３２および負極活物質層３７間の絶縁を確実に得ることができる。   According to the laminated battery 10 configured as described above, even if the positive electrode active material layer 32 may be missing by covering the negative electrode active material layer 37 with the electrolyte layer 41, the positive electrode through the missing portion. It is possible to prevent the active material layer 32 and the negative electrode active material layer 37 from being short-circuited. In addition, since the electrolyte layer 41 is provided so as to cover only the negative electrode active material layer 37 of the negative electrode active material layer 37 and the negative electrode current collector foil 36, it is possible to prevent the electrolyte layer 41 from being excessively bent. Thereby, breakage of the electrolyte layer 41 can be prevented, and insulation between the positive electrode active material layer 32 and the negative electrode active material layer 37 can be reliably obtained.

なお、本実施の形態では、電解質層４１によって負極活物質層３７が覆われた場合について説明したが、負極活物質層３７に替えて正極活物質層３２が覆われても良い。また、積層型電池１０は、リチウムイオン電池に限定されず、リチウムイオン電池以外の２次電池から形成されても良い。   In this embodiment, the case where the negative electrode active material layer 37 is covered with the electrolyte layer 41 has been described. However, the positive electrode active material layer 32 may be covered instead of the negative electrode active material layer 37. The stacked battery 10 is not limited to a lithium ion battery, and may be formed from a secondary battery other than a lithium ion battery.

また、積層型電池１０を、燃料電池と２次電池とを駆動源とする燃料電池ハイブリッド車両（ＦＣＨＶ：Fuel Cell Hybrid Vehicle）または電気自動車（ＥＶ：Electric Vehicle）に搭載することもできる。本実施の形態におけるハイブリッド車両では、燃費最適動作点で内燃機関を駆動するのに対して、燃料電池ハイブリッド車両では、発電効率最適動作点で燃料電池を駆動する。また、２次電池の使用に関しては、両方のハイブリッド車両で基本的に変わらない。   In addition, the stacked battery 10 can be mounted on a fuel cell hybrid vehicle (FCHV) or an electric vehicle (EV) using a fuel cell and a secondary battery as drive sources. In the hybrid vehicle in the present embodiment, the internal combustion engine is driven at the fuel efficiency optimum operating point, whereas in the fuel cell hybrid vehicle, the fuel cell is driven at the power generation efficiency optimum operating point. The use of the secondary battery is basically the same for both hybrid vehicles.

図１１は、図２中の単電池の変形例を示す断面図である。図１１を参照して、本変形例では、正極活物質層３２および負極活物質層３７の双方が、電解質層４１によって覆われている。本変形例における積層型電池の製造方法は、正極活物質層３２を覆うように、正極集電箔３１の表面３１ａ上に電解質層４１を形成する工程をさらに備える。正極集電箔３１の表面３１ａ上および負極集電箔３６の表面３６ａ上に電解質層４１を形成する工程の後、負極集電箔３６と正極集電箔３１とを積層する。   FIG. 11 is a cross-sectional view showing a modification of the unit cell in FIG. Referring to FIG. 11, in this modification, both positive electrode active material layer 32 and negative electrode active material layer 37 are covered with electrolyte layer 41. The method for manufacturing a stacked battery in this modification further includes a step of forming an electrolyte layer 41 on the surface 31 a of the positive electrode current collector foil 31 so as to cover the positive electrode active material layer 32. After the step of forming the electrolyte layer 41 on the surface 31 a of the positive electrode current collector foil 31 and on the surface 36 a of the negative electrode current collector foil 36, the negative electrode current collector foil 36 and the positive electrode current collector foil 31 are laminated.

このような構成によれば、電解質層４１によって、正極活物質層３２および負極活物質層３７が欠落することを防止できる。これにより、積層型電池１０の電池容量が低下することを防止できる。また、正極集電箔３１および負極集電箔３６のいずれか一方に設けられた電解質層４１にピンホールが形成されることがあっても、負極集電箔３６と正極集電箔３１とを積層する時に、正極集電箔３１および負極集電箔３６のいずれか他方に設けられた電解質層４１によって、そのピンホールを塞ぐことができる。これにより、正極および負極間の短絡をより確実に防ぐことができる。   According to such a configuration, the electrolyte layer 41 can prevent the positive electrode active material layer 32 and the negative electrode active material layer 37 from being lost. Thereby, it can prevent that the battery capacity of the laminated battery 10 falls. Even if pinholes may be formed in the electrolyte layer 41 provided on either the positive electrode current collector foil 31 or the negative electrode current collector foil 36, the negative electrode current collector foil 36 and the positive electrode current collector foil 31 At the time of lamination, the pinhole can be closed by the electrolyte layer 41 provided on the other of the positive electrode current collector foil 31 and the negative electrode current collector foil 36. Thereby, the short circuit between a positive electrode and a negative electrode can be prevented more reliably.

（実施の形態２）
図１２は、この発明の実施の形態２における積層型電池を示す断面図である。図１２を参照して、本実施の形態における積層型電池は、正極活物質層３２および負極活物質層３７が１枚の集電箔６１に設けられるバイポーラ２次電池である。 (Embodiment 2)
FIG. 12 is a cross-sectional view showing a stacked battery according to Embodiment 2 of the present invention. Referring to FIG. 12, the stacked battery in the present embodiment is a bipolar secondary battery in which positive electrode active material layer 32 and negative electrode active material layer 37 are provided on one current collecting foil 61.

互いに隣り合う単電池３０を、それぞれ単電池３０ｍおよび単電池３０ｎと呼ぶことにすると、単電池３０ｍの正極活物質層３２が、集電箔６１の表面６１ａ上に形成され、単電池３０ｎの負極活物質層３７が、集電箔６１の裏面６１ｂ上に形成されている。   When the unit cells 30 adjacent to each other are referred to as the unit cell 30m and the unit cell 30n, respectively, the positive electrode active material layer 32 of the unit cell 30m is formed on the surface 61a of the current collector foil 61, and the negative electrode of the unit cell 30n. An active material layer 37 is formed on the back surface 61 b of the current collector foil 61.

この発明の実施の形態２における積層型電池は、積層された第１および第２の集電体としての２枚の集電箔６１（以降、集電箔６１ｐおよび集電箔６１ｑと呼ぶ）と、正極および負極のいずれか一方としての負極をなす第１の活物質層としての負極活物質層３７と、正極および負極のいずれか他方としての正極をなす第２の活物質層としての正極活物質層３２と、負極活物質層３７と正極活物質層３２との間に配置された固体電解質としての電
解質層４１とを備える。集電箔６１ｐは、第１の表面としての表面６１ｂを有し、集電箔６１ｑは、第２の表面としての表面６１ａを有する。表面６１ｂと表面６１ａとは互いに向い合う。負極活物質層３７は、表面６１ｂ上に形成されている。正極活物質層３２は、負極活物質層３７と対向し、表面６１ａ上に形成されている。電解質層４１の端部４１ｕは、表面６１ｂ上に接触する。負極活物質層３７は、電解質層４１によって覆われている。 A laminated battery according to Embodiment 2 of the present invention includes two current collecting foils 61 (hereinafter referred to as current collecting foil 61p and current collecting foil 61q) as first and second current collectors laminated. , A negative electrode active material layer 37 as a first active material layer forming a negative electrode as one of the positive electrode and the negative electrode, and a positive electrode active as a second active material layer forming a positive electrode as the other of the positive electrode and the negative electrode A material layer 32 and an electrolyte layer 41 as a solid electrolyte disposed between the negative electrode active material layer 37 and the positive electrode active material layer 32 are provided. The current collector foil 61p has a surface 61b as a first surface, and the current collector foil 61q has a surface 61a as a second surface. The surface 61b and the surface 61a face each other. The negative electrode active material layer 37 is formed on the surface 61b. The positive electrode active material layer 32 faces the negative electrode active material layer 37 and is formed on the surface 61a. The end portion 41u of the electrolyte layer 41 is in contact with the surface 61b. The negative electrode active material layer 37 is covered with an electrolyte layer 41.

このように構成された、この発明の実施の形態２における積層型電池によれば、実施の形態１に記載の効果と同様の効果を得ることができる。   According to the stacked battery in the second embodiment of the present invention configured as described above, the same effects as those described in the first embodiment can be obtained.

なお、実施の形態２におけるバイポーラ２次電池からなる積層型電池に、実施の形態１において説明した各変形例を適用しても良い。   Each modification described in the first embodiment may be applied to the stacked battery including the bipolar secondary battery in the second embodiment.

今回開示された実施の形態はすべての点で例示であって制限的なものではないと考えられるべきである。本発明の範囲は上記した説明ではなくて特許請求の範囲によって示され、特許請求の範囲と均等の意味および範囲内でのすべての変更が含まれることが意図される。   The embodiment disclosed this time should be considered as illustrative in all points and not restrictive. The scope of the present invention is defined by the terms of the claims, rather than the description above, and is intended to include any modifications within the scope and meaning equivalent to the terms of the claims.

この発明の実施の形態１における積層型電池を示す断面図である。It is sectional drawing which shows the laminated battery in Embodiment 1 of this invention. 図１中の積層型電池が備える単電池を示す断面図である。It is sectional drawing which shows the single battery with which the laminated battery in FIG. 1 is provided. 図２中の単電池を構成する負極を示す斜視図である。It is a perspective view which shows the negative electrode which comprises the single battery in FIG. 図２中の単電池の製造方法の第１の正極形成工程を示す断面図である。FIG. 3 is a cross-sectional view showing a first positive electrode forming step in the method for manufacturing the unit cell in FIG. 2. 図２中の単電池の製造方法の第２の正極形成工程を示す断面図である。It is sectional drawing which shows the 2nd positive electrode formation process of the manufacturing method of the single battery in FIG. 図２中の単電池の製造方法の第１の負極形成工程を示す断面図である。FIG. 3 is a cross-sectional view showing a first negative electrode forming step of the method for manufacturing the unit cell in FIG. 2. 図２中の単電池の製造方法の第２の負極形成工程を示す断面図である。It is sectional drawing which shows the 2nd negative electrode formation process of the manufacturing method of the cell in FIG. 図２中の単電池の製造方法の積層工程を示す断面図である。It is sectional drawing which shows the lamination process of the manufacturing method of the single battery in FIG. 図２中の単電池の製造方法の切断工程を示す断面図である。It is sectional drawing which shows the cutting process of the manufacturing method of the single battery in FIG. 図４および図５中に示す工程を経て得られた正極集電箔を示す斜視図である。It is a perspective view which shows the positive electrode current collection foil obtained through the process shown in FIG. 4 and FIG. 図２中の単電池の変形例を示す断面図である。It is sectional drawing which shows the modification of the single battery in FIG. この発明の実施の形態２における積層型電池を示す断面図である。It is sectional drawing which shows the laminated battery in Embodiment 2 of this invention.

符号の説明Explanation of symbols

１０ 積層型電池、３１ 正極集電箔、３１ａ，３６ａ，６１ａ，６１ｂ 表面、３２
正極活物質層、３６ 負極集電箔、３７ 負極活物質層、４１ 電解質層、４１ｕ 端部、６１ｐ，６１ｑ 集電箔、２００，３００，４００ 領域。 10 laminated battery, 31 positive electrode current collector foil, 31a, 36a, 61a, 61b surface, 32
Positive electrode active material layer, 36 negative electrode current collector foil, 37 negative electrode active material layer, 41 electrolyte layer, 41u end, 61p, 61q current collector foil, 200, 300, 400 region.

Claims (3)

互いに向い合う第１および第２の表面をそれぞれ有し、積層された第１および第２の集電体と、
前記第１の表面上に形成され、正極および負極のいずれか一方をなす第１の活物質層と、
前記第２の表面上に形成され、前記第１の活物質層と対向し、正極および負極のいずれか他方をなす第２の活物質層と、
前記第１の活物質層と前記第２の活物質層との間に配置された固体電解質とを備え、
前記固体電解質の端部は、前記第１の表面上に接触し、前記第１の活物質層は、前記固体電解質によって覆われている、積層型電池。 First and second current collectors having first and second surfaces facing each other and stacked;
A first active material layer formed on the first surface and forming one of a positive electrode and a negative electrode;
A second active material layer formed on the second surface, facing the first active material layer and forming either the positive electrode or the negative electrode;
A solid electrolyte disposed between the first active material layer and the second active material layer;
An end portion of the solid electrolyte is in contact with the first surface, and the first active material layer is covered with the solid electrolyte. 前記第２の活物質層は、前記固体電解質によって覆われている、請求項１に記載の積層型電池。   The stacked battery according to claim 1, wherein the second active material layer is covered with the solid electrolyte. 請求項１または２に記載の積層型電池の製造方法であって、
前記第１および第２の表面上に、それぞれ前記第１および第２の活物質層を形成する工程と、
前記第１の活物質層を覆うように、前記第１の表面上に前記固体電解質を形成する工程と、
前記固体電解質を形成する工程の後、前記第１の集電体と前記第２の集電体とを積層する工程とを備える、積層型電池の製造方法。 It is a manufacturing method of the lamination type battery according to claim 1 or 2,
Forming the first and second active material layers on the first and second surfaces, respectively;
Forming the solid electrolyte on the first surface so as to cover the first active material layer;
After the step of forming the solid electrolyte, a method of manufacturing a stacked battery, comprising: stacking the first current collector and the second current collector.
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