JP7289659B2 - Housing structure of all-solid-state battery and module structure using the same - Google Patents

Housing structure of all-solid-state battery and module structure using the same Download PDF

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JP7289659B2
JP7289659B2 JP2019013560A JP2019013560A JP7289659B2 JP 7289659 B2 JP7289659 B2 JP 7289659B2 JP 2019013560 A JP2019013560 A JP 2019013560A JP 2019013560 A JP2019013560 A JP 2019013560A JP 7289659 B2 JP7289659 B2 JP 7289659B2
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武典 橋本
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Hyundai Motor Co
Kia Corp
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    • H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/116—Primary casings; Jackets or wrappings characterised by the material
    • 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
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    • H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
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    • 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
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0564—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of organic materials only
    • H01M10/0565—Polymeric materials, e.g. gel-type or solid-type
    • 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
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/058—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
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • 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
    • H01M50/10—Primary casings; Jackets or wrappings
    • H01M50/102—Primary casings; Jackets or wrappings characterised by their shape or physical structure
    • H01M50/112—Monobloc comprising multiple compartments
    • 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
    • H01M50/20—Mountings; Secondary casings or frames; Racks, modules or packs; Suspension devices; Shock absorbers; Transport or carrying devices; Holders
    • H01M50/258—Modular batteries; Casings provided with means for assembling
    • 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
    • H01M50/502—Interconnectors for connecting terminals of adjacent batteries; Interconnectors for connecting cells outside a battery casing
    • 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
    • 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
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    • 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
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Description

本発明は、全固体電池の筐体構造及びこれを用いたモジュール構造に関し、特に固体電池素子を複数直列に積層した固体電池積層体とこれを挟み込んで外部端子となる正負の電極プレートとの外周部を樹脂封止して一体化することでスペース効率を高めた全固体電池の筐体構造及びこれを用いたモジュール構造に関する。 The present invention relates to a housing structure of an all-solid-state battery and a module structure using the same, and in particular, the outer periphery of a solid-state battery stack in which a plurality of solid-state battery elements are stacked in series and positive and negative electrode plates sandwiching the stack and serving as external terminals. The present invention relates to a housing structure of an all-solid-state battery in which space efficiency is improved by resin-sealing and integrating parts, and a module structure using the same.

様々な場面で充電可能な２次電池が幅広く採用されている。特に高信頼性が求められる自動車分野においてもガソリンエンジンからモータへと駆動系の転換が進んでおり、これに伴い２次電池の搭載車両も増えつつある。こうした２次電池は電気的な性能の他にも移動を伴う用途では小型・軽量化が求められ、現時点ではリチウムイオン電池が多く使われてきている。 Rechargeable secondary batteries are widely used in various situations. Especially in the field of automobiles, where high reliability is required, the conversion of drive systems from gasoline engines to motors is progressing, and along with this, the number of vehicles equipped with secondary batteries is increasing. In addition to electrical performance, such secondary batteries are required to be small and lightweight for applications involving movement, and at present, lithium-ion batteries are often used.

リチウムイオン電池は性能もよく使い勝手がよい反面、有機溶剤系の電解液を使用するために機械的な衝撃等により短絡が生じると発火事故に至ることから安全性には課題があることが知られている。このため信頼性が求められる用途では様々な安全対策や品質管理に十分配慮しながら使用されている。
このようなリチウムイオン電池の安全性の課題を解決するために電解液の代わりに固体の電解質を使用する全固体電池の開発が進められている。 Lithium-ion batteries have good performance and are easy to use, but because they use an organic solvent-based electrolyte, it is known that there is a safety issue because if a short circuit occurs due to mechanical shock, etc., it will lead to a fire accident. ing. For this reason, in applications that require reliability, they are used with due consideration given to various safety measures and quality control.
In order to solve the safety problem of lithium-ion batteries, development of all-solid-state batteries using solid electrolytes instead of electrolytic solutions is underway.

特許文献１には負極集電タブを有する負極集電体層、負極活物質層、固体電解質層、正極活物質層、及び正極集電タブを有する正極集電体層がこの順に積層された全固体電池素子を従来のリチウムイオン電池と同様にラミネートフィルムからなる外装体に収容し、積層方向に加圧しながら充填剤を充填して封入するラミネート全固体電池の製造方法が開示されている。 Patent Document 1 discloses a total structure in which a negative electrode current collector layer having a negative electrode current collecting tab, a negative electrode active material layer, a solid electrolyte layer, a positive electrode active material layer, and a positive electrode current collector layer having a positive electrode current collecting tab are laminated in this order. A method for producing a laminated all-solid-state battery is disclosed, in which a solid-state battery element is housed in an outer package made of a laminate film in the same manner as a conventional lithium-ion battery, and a filler is filled and sealed while applying pressure in the stacking direction.

特許文献２には正極層と、固体電解質膜と、負極層とがこの順に積層された発電ユニットがバイポーラ層を挟んで複数積層された発電要素を電池ケースに収納し流動性封止剤で封止した固体型電池が開示されている。 In Patent Document 2, a power generation unit in which a positive electrode layer, a solid electrolyte membrane, and a negative electrode layer are laminated in this order is housed in a battery case and sealed with a fluid sealant. A stationary solid state battery is disclosed.

特許文献１の全固体電池も特許文献２の固体型電池も、ともに電池の外部端子は集電体から延長されるか又は集電体と平行に引き出されたタブとして形成されており、自動車などのように、高電圧を要するためにこれらの電池を直列接続してモジュールとして使用する場合、タブ同士を接続する接続エリアが必要となり無駄なスペースをとることとなる。
そこで直列接続のための無駄なスペースを取らないでモジュール化が可能な全固体電池の筐体構造が求められる。 In both the all-solid-state battery of Patent Document 1 and the solid-state battery of Patent Document 2, the external terminal of the battery is formed as a tab extended from the current collector or pulled out in parallel with the current collector. When these batteries are used as a module by connecting them in series because they require a high voltage, a connection area for connecting the tabs is required, resulting in wasted space.
Therefore, there is a demand for a housing structure for all-solid-state batteries that can be modularized without taking up unnecessary space for series connection.

特開２０１８－１３３１７５号公報JP 2018-133175 A 特開２００９－２５２５４８号公報JP 2009-252548 A

本発明は、上記従来の全固体電池における問題点に鑑みてなされたものであって、本発明の目的は、固体電池素子を複数直列に積層した固体電池積層体とこれを挟み込んで外部端子となる正負の電極プレートとの外周部を樹脂封止して一体化することでスペース効率を高めた全固体電池の筐体構造及びこれを用いたモジュール構造を提供するところにある。 The present invention has been made in view of the problems in the conventional all-solid-state battery described above. An object of the present invention is to provide a housing structure for an all-solid-state battery in which space efficiency is improved by integrating the positive and negative electrode plates by resin-sealing the outer periphery thereof, and a module structure using the same.

上記目的を達成するためになされた本発明による全固体電池の筐体構造は、集電体の片面に正極を形成した正極電極と、正極電極と対向し集電体の正極と対向する面に負極を形成した負極電極と、正極電極と負極電極との間に位置する複数の固体電解質と、隣接する複数の固体電解質の間にそれぞれ位置して集電体の片面に正極を形成し正極と反対側の面に負極を形成した複数のバイポーラ電極とを備える固体電池積層体と、前記正極電極に隣接して配置された正電極プレートと、前記負極電極に隣接して配置された負電極プレートと、前記固体電池積層体、前記正電極プレート、及び前記負電極プレートの外周部を覆い、前記正電極プレート、及び前記負電極プレートの電極面が露出するように一体化する樹脂筐体とを有し、前記樹脂筐体は樹脂成型金型内で前記正電極プレートと、前記負電極プレートとを前記固体電池積層体に押し付ける加圧状態で注入されて固化されることで加圧状態を保ちつつ前記固体電池積層体を封止することを特徴とする。 The housing structure of the all-solid-state battery according to the present invention, which has been made to achieve the above object, comprises a positive electrode in which a positive electrode is formed on one side of a current collector, and a surface facing the positive electrode and facing the positive electrode of the current collector. A negative electrode forming a negative electrode, a plurality of solid electrolytes positioned between the positive electrode and the negative electrode, and a positive electrode formed on one side of a current collector positioned between the adjacent solid electrolytes. A solid battery stack comprising a plurality of bipolar electrodes with negative electrodes formed on opposite surfaces, a positive electrode plate positioned adjacent to the positive electrodes, and a negative electrode plate positioned adjacent to the negative electrodes. and a resin casing that covers the solid battery stack, the positive electrode plate, and the negative electrode plate, and integrates them so that the electrode surfaces of the positive electrode plate and the negative electrode plate are exposed. The resin casing is injected in a resin molding die in a pressurized state that presses the positive electrode plate and the negative electrode plate against the solid battery stack, and is solidified to maintain the pressurized state. and sealing the solid battery stack.

上記目的を達成するためになされた本発明による全固体電池のモジュール構造は、全固体電池の筐体構造を電気的に複数接続するモジュール構造であって、前記全固体電池の筐体構造は、集電体の片面に正極を形成した正極電極と、正極電極と対向し集電体の正極と対向する面に負極を形成した負極電極と、正極電極と負極電極との間に位置する複数の固体電解質と、隣接する複数の固体電解質の間にそれぞれ位置して集電体の片面に正極を形成し正極と反対側の面に負極を形成した複数のバイポーラ電極とを備える固体電池積層体と、前記正極電極に隣接して配置された正電極プレートと、前記負極電極に隣接して配置された負電極プレートと、前記固体電池積層体、前記正電極プレート、及び前記負電極プレートの外周部を覆い、前記正電極プレート、及び前記負電極プレートの電極面が露出するように一体化する樹脂筐体とを有し、前記樹脂筐体は樹脂成型金型内で前記正電極プレートと、前記負電極プレートとを前記固体電池積層体に押し付ける加圧状態で注入されて固化されることで加圧状態を保ちつつ前記固体電池積層体を封止し、前記複数の全固体電池の筐体構造は露出する正電極プレートが、他の全固体電池の筐体構造の露出する負電極プレートと隣接するように直列に配列されることを特徴とする。 A module structure for an all-solid-state battery according to the present invention, which has been made to achieve the above object, is a module structure for electrically connecting a plurality of casing structures of an all-solid-state battery, wherein the casing structure for the all-solid-state battery comprises: A positive electrode having a positive electrode formed on one side of a current collector, a negative electrode facing the positive electrode and having a negative electrode formed on a side of the current collector facing the positive electrode, and a plurality of electrodes positioned between the positive electrode and the negative electrode. A solid battery stack comprising a solid electrolyte and a plurality of bipolar electrodes positioned between a plurality of adjacent solid electrolytes, each having a positive electrode formed on one side of a current collector and a negative electrode formed on the opposite side of the positive electrode. , a positive electrode plate arranged adjacent to the positive electrode; a negative electrode plate arranged adjacent to the negative electrode; outer peripheral portions of the solid battery stack, the positive electrode plate, and the negative electrode plate; and a resin housing integrated with the positive electrode plate and the negative electrode plate so that the electrode surfaces of the positive electrode plate and the negative electrode plate are exposed, and the resin housing includes the positive electrode plate and the The solid battery stack is sealed while maintaining the pressurized state by being injected and solidified in a pressurized state that presses the negative electrode plate against the solid battery stack, and the housing structure of the plurality of all-solid-state batteries is characterized in that the exposed positive electrode plates are arranged in series adjacent to the exposed negative electrode plates of other all-solid-state battery housing structures.

前記対向する正電極プレートと負電極プレートとは導電性材料を挟んで互いに接続され、前記導電性材料は柔軟性を有する導電性板状部材又は導電性フィルム材、或は導電性のペースト材であることが好ましい。 The positive electrode plate and the negative electrode plate facing each other are connected to each other with a conductive material sandwiched therebetween, and the conductive material is a flexible conductive plate-like member, a conductive film material, or a conductive paste material. Preferably.

本発明に係る全固体電池の筐体構造によれば、固体電池積層体を挟み込んで樹脂筐体により一体化される正負の電極プレートは全固体電池の筐体構造の外部端子として機能するため、全固体電池の筐体構造の正電極プレートを他の全固体電池の筐体構造の負電極プレートと接触させるようにして直列に複数個配置することにより、電気的に直列接続することができ、余分な接続領域を必要としないスペース効率の高いモジュール構造を容易に実現することが可能となる。更に従来方式のタブによる電極構造と異なりタブ同士の結線の必要がないことから結線に係る工数を低減することもできる。 According to the case structure of the all-solid-state battery according to the present invention, the positive and negative electrode plates integrated by the resin case sandwiching the solid-state battery stack function as external terminals of the case structure of the all-solid-state battery. By arranging a plurality of positive electrode plates of the housing structure of the all-solid-state battery in series so as to be in contact with the negative electrode plate of the housing structure of another all-solid-state battery, they can be electrically connected in series, It is possible to easily realize a highly space-efficient module structure that does not require an extra connection area. Furthermore, unlike the conventional electrode structure using tabs, since there is no need to connect tabs to each other, man-hours for connection can be reduced.

また、本発明に係る全固体電池の筐体構造によれば、固体電池積層体は積層方向に加圧された状態で外周部を樹脂筐体で封止されて拘束されるため、固体電池積層体が充放電を行う使用状態で膨張するのを抑制することが可能である。 Further, according to the case structure of the all-solid-state battery according to the present invention, the solid-state battery stack is constrained by sealing the outer peripheral portion with the resin case while being pressed in the stacking direction. It is possible to suppress the expansion of the body in the state of use in which charging and discharging are performed.

本発明に係る全固体電池の筐体構造を用いたモジュール構造によれば、直列接続する全固体電池の筐体構造の電極プレート間に柔軟性を有する導電性板状部材又は導電性フィルム材、或は導電性のペースト材を挟んで互いに接続されるため隣接する全固体電池の筐体構造の電極プレート同士の密着性が向上し、電気的な接触抵抗を低減するとともに熱抵抗も低減され、電気特性、熱特性の優れたモジュール構造が実現可能である。 According to the module structure using the housing structure of the all-solid-state battery according to the present invention, a conductive plate-like member or a conductive film material having flexibility between the electrode plates of the housing structure of the all-solid-state battery connected in series, Alternatively, since they are connected to each other with a conductive paste material sandwiched between them, the adhesion between the electrode plates of the casing structure of the adjacent all-solid-state battery is improved, the electrical contact resistance is reduced, and the thermal resistance is also reduced. A module structure with excellent electrical and thermal properties can be realized.

本発明の一実施形態による全固体電池の筐体構造を部分的に切断して内部構造が見えるように示す斜視図である。1 is a perspective view showing the internal structure by partially cutting the housing structure of an all-solid-state battery according to an embodiment of the present invention; FIG. 図１に示す全固体電池の筐体構造の内部構造を水平断面により概略的に示す図である。2 is a schematic horizontal cross-sectional view of the internal structure of the housing structure of the all-solid-state battery shown in FIG. 1; FIG. 本発明の一実施形態によるモジュール構造を概略的に示す図である。Fig. 3 schematically shows a module structure according to an embodiment of the present invention; 図３に示すモジュール構造の内部構造を水平断面により概略的に示す図である。4 is a diagram schematically showing the internal structure of the module structure shown in FIG. 3 in a horizontal section; FIG. 本発明の一実施形態によるモジュール構造の締結方法を概略的に示す図である。Fig. 3 schematically illustrates a method of fastening a modular structure according to an embodiment of the present invention; 図５に示すモジュール構造の内部構造を水平断面により概略的に示す図である。FIG. 6 is a diagram schematically showing the internal structure of the module structure shown in FIG. 5 in a horizontal section;

次に、本発明に係る全固体電池の筐体構造及びこれを用いたモジュール構造を実施するための形態の具体例を、図面を参照しながら詳細に説明する。
図１は、本発明の一実施形態による全固体電池の筐体構造を部分的に切断して内部構造が見えるように示す斜視図である。 Next, a specific example of a form for implementing a housing structure of an all-solid-state battery and a module structure using the same according to the present invention will be described in detail with reference to the drawings.
FIG. 1 is a perspective view showing the internal structure by partially cutting the housing structure of an all-solid-state battery according to one embodiment of the present invention.

図１を参照すると、本発明の一実施形態による全固体電池の筐体構造１は充放電を行う固体電池積層体２０と、固体電池積層体２０を挟み込むように位置する正電極プレート３０及び負電極プレート４０と、固体電池積層体２０並びに正電極プレート３０及び負電極プレート４０の外周部を覆って全体を一体化する樹脂筐体５０とを含む。 Referring to FIG. 1, a housing structure 1 for an all-solid-state battery according to an embodiment of the present invention includes a solid-state battery stack 20 for charging and discharging, a positive electrode plate 30 and a negative electrode plate 30 sandwiching the solid-state battery stack 20 . It includes an electrode plate 40, and a resin casing 50 that covers the solid battery stack 20, the positive electrode plate 30, and the negative electrode plate 40, and integrates the whole.

正電極プレート３０及び負電極プレート４０は片面が樹脂筐体５０で覆われる外周部を除いて外部に露出し、この露出した部分が外部への電極面として機能するように構成されている。即ち全固体電池の筐体構造１は全体が略直方体として形成され、全固体電池の筐体構造１の１側面に露出する正電極プレート３０の電極面が正電極、正電極と対向する面に露出する負電極プレート４０の電極面が負電極となり、この正電極と負電極が全固体電池の筐体構造１の外部端子となる。 The positive electrode plate 30 and the negative electrode plate 40 are exposed to the outside except for the outer peripheral portion covered with the resin housing 50 on one side, and the exposed portion functions as an electrode surface to the outside. That is, the entire solid-state battery housing structure 1 is formed as a substantially rectangular parallelepiped. The exposed electrode surface of the negative electrode plate 40 serves as a negative electrode, and the positive electrode and the negative electrode serve as external terminals of the housing structure 1 of the all-solid-state battery.

図２は、図１に示す全固体電池の筐体構造の内部構造を水平断面により概略的に示す図である。
図２を参照すると、固体電池積層体２０は集電体２１の片面に正極２２を形成した正極電極２３、正極電極２３の反対側に位置し、集電体２１の正極２２と対向する面に負極２４を形成した負極電極２５、正極電極２３と負極電極２５との間に位置する複数の固体電解質２６、及び隣接する複数の固体電解質２６の間にそれぞれ位置して集電体２１の片面に正極２２を形成し正極２２と反対側の面に負極２４を形成した複数のバイポーラ電極２７とを備える。 FIG. 2 is a diagram schematically showing the internal structure of the housing structure of the all-solid-state battery shown in FIG. 1 by a horizontal cross section.
Referring to FIG. 2, the solid battery stack 20 includes a positive electrode 23 having a positive electrode 22 formed on one side of a current collector 21, a positive electrode 23 located on the opposite side of the positive electrode 23, and a surface of the current collector 21 facing the positive electrode 22. A negative electrode 25 forming a negative electrode 24, a plurality of solid electrolytes 26 positioned between the positive electrode 23 and the negative electrode 25, and a plurality of adjacent solid electrolytes 26 positioned on one side of the current collector 21, respectively. It comprises a plurality of bipolar electrodes 27 forming positive electrodes 22 and forming negative electrodes 24 on the surface opposite to the positive electrodes 22 .

このように固体電池積層体２０は複数の層が積層されて構成されるが、部分的にみると正極２２、固体電解質２６、負極２４がこの順に組み合わされた固体電池としての最小単位構造が直列に複数配列された構造となっている。
ここで固体電池積層体２０に使用する材料は固体電池として機能する材料であればその種類や組合せに制限はない。固体電池積層体２０のそれぞれの層には以下のような公知の材料が使用される。 As described above, the solid battery laminate 20 is configured by laminating a plurality of layers. It has a structure in which multiple arrays are arranged in
The materials used for the solid-state battery stack 20 are not limited in kind and combination as long as they function as solid-state batteries. The following known materials are used for each layer of the solid battery stack 20 .

集電体２１は、一般には金属箔が使用され、金属箔の材料としてはＡｌ、ＳＵＳ、Ｃｕ、Ｎｉなどの材料が使用される。固体電池積層体２０には正極電極２３、負極電極２５、バイポーラ電極２７の３種類の電極にそれぞれ集電体２１を含むが、３種類の電極の材料は同じでもよいし、異なる材料でもよい。 A metal foil is generally used for the current collector 21, and materials such as Al, SUS, Cu, and Ni are used as materials for the metal foil. The solid battery stack 20 includes current collectors 21 for three types of electrodes, a positive electrode 23, a negative electrode 25, and a bipolar electrode 27, and the materials of the three types of electrodes may be the same or different.

正極２２は、正極活性物質を含み、正極活性物質としてはＬｉＣｏＯ２、ＬｉＭｎＯ２、ＬｉＭｎ２Ｏ４、ＬｉＦｅＰＯ４、ＬｉＭｎＰＯ４等が挙げられる。正極は正極電極２３とバイポーラ電極２７とに含まれるが、正極電極２３とバイポーラ電極２７とで同一の正極活性物質を使用するのが好ましい。 The positive electrode 22 contains a positive electrode active material such as LiCoO 2 , LiMnO 2 , LiMn 2 O 4 , LiFePO 4 , LiMnPO 4 and the like. The positive electrode is included in the positive electrode 23 and the bipolar electrode 27, and it is preferable that the positive electrode 23 and the bipolar electrode 27 use the same positive electrode active material.

負極２４は、負極活性物質を含み、負極活性物質としてはグラファイト、ハードカーボン、ソフトカーボンなどの炭素材料や、Ｌｉ４Ｔｉ５Ｏ１２等の無機酸化物が使用される。負極は負極電極２５とバイポーラ電極２７とに含まれるが、負極電極２５とバイポーラ電極２７とで同一の負極活性物質を使用するのが好ましい。 The negative electrode 24 contains a negative electrode active material, and carbon materials such as graphite, hard carbon, and soft carbon, and inorganic oxides such as Li 4 Ti 5 O 12 are used as the negative electrode active material. The negative electrode is included in the negative electrode 25 and the bipolar electrode 27, and it is preferable that the negative electrode 25 and the bipolar electrode 27 use the same negative electrode active material.

固体電解質２６の材料としては、酸化物系固体電解質や硫化物系固体電解質が使用され、酸化物系固体電解質としては、Ｌｉ１．５Ａｌ０．５Ｔｉ１．５（ＰＯ４）３、Ｌｉ０．５Ｌａ０．５ＴｉＯ３等が挙げられ、硫化物系固体電解質としては、Ｌｉ２Ｓ－Ｐ２Ｓ５、Ｌｉ２Ｓ－ＳｉＳ２、ＬｉＧｅ０．２５Ｐ０．７５Ｓ４等が挙げられる。 As a material for the solid electrolyte 26, an oxide-based solid electrolyte or a sulfide - based solid electrolyte is used . 0.5 La 0.5 TiO 3 and the like, and sulfide-based solid electrolytes include Li 2 SP 2 S 5 , Li 2 S—SiS 2 , LiGe 0.25 P 0.75 S 4 and the like. mentioned.

固体電池積層体２０に加え、正極電極２３の外側面に隣接して正電極プレート３０が配置され、負極電極２５の外側面に隣接して負電極プレート４０が配置され、固体電池積層体２０、正電極プレート３０、及び負電極プレート４０の外周部が樹脂筐体５０によって覆われ一体化される。このとき外周部を覆う樹脂筐体５０が正電極プレート３０及び負電極プレート４０の電極面より高く突出しないように正電極プレート３０及び負電極プレート４０の樹脂筐体５０に覆われる部分は部分的に薄くした段差構造としている。 In addition to the solid battery stack 20, a positive electrode plate 30 is arranged adjacent to the outer surface of the positive electrode 23, a negative electrode plate 40 is arranged adjacent to the outer surface of the negative electrode 25, and the solid battery stack 20, The outer peripheral portions of the positive electrode plate 30 and the negative electrode plate 40 are covered with a resin housing 50 and integrated. At this time, the portions of the positive electrode plate 30 and the negative electrode plate 40 covered with the resin housing 50 are partially covered so that the resin housing 50 covering the outer peripheral portion does not protrude higher than the electrode surfaces of the positive electrode plate 30 and the negative electrode plate 40. It has a thin step structure.

正電極プレート３０及び負電極プレート４０は、金属材料など電気伝導性に加え熱伝導性の良い材料で形成される。露出する電極面には耐食性を向上させたり接触抵抗を低く保たせたりするためのメッキ処理などの表面処理を施してもよい。
樹脂筐体５０は以下に示すように金型に注入し硬化させて形成するものであり、熱硬化型の樹脂を使用する。樹脂筐体５０は全固体電池の筐体構造１を構造体としてまとめるためのものであり、強度と耐環境性が求められる。そこでエポキシ系の封止材料などの熱硬化型の樹脂を使用する。 The positive electrode plate 30 and the negative electrode plate 40 are made of a material having good thermal conductivity in addition to electrical conductivity, such as a metallic material. The exposed electrode surface may be subjected to surface treatment such as plating for improving corrosion resistance and keeping contact resistance low.
The resin casing 50 is formed by injecting it into a mold and curing it as described below, and uses a thermosetting resin. The resin housing 50 is for putting together the housing structure 1 of the all-solid-state battery as a structural body, and is required to have strength and environmental resistance. Therefore, a thermosetting resin such as an epoxy sealing material is used.

図１、２に示す全固体電池の筐体構造１を形成する場合、図２に示すように正電極プレート３０、固体電池積層体２０、負電極プレート４０をこの順に重ね合わせた組み合わせ構造体を、モールド金型に収納し、モールド金型の型締めの際、組み合わせ構造体に積層方向の圧力が加わるようにモールド金型の深さを調整し、型締めによって圧力が加わった状態で熱硬化型の樹脂を外周部に注入して金型内で硬化させる。 When forming the housing structure 1 of the all-solid-state battery shown in FIGS. , The mold is placed in a mold, and when the mold is clamped, the depth of the mold is adjusted so that pressure is applied to the combined structure in the stacking direction. The mold resin is injected into the outer periphery and cured in the mold.

このように加圧状態で樹脂封止することにより、正電極プレート３０、固体電池積層体２０、負電極プレート４０の間の接触抵抗を下げ、電池としての性能の低下を防ぐことが可能である。また樹脂筐体により加圧状態で保持するように固めることにより、固体電池積層体２０が充放電時に膨張するのを抑えることが可能となる。 By resin-sealing in a pressurized state in this way, it is possible to reduce the contact resistance between the positive electrode plate 30, the solid battery stack 20, and the negative electrode plate 40, and prevent deterioration in battery performance. . Further, by solidifying the solid battery stack 20 so as to be held in a pressurized state by the resin casing, it is possible to suppress expansion of the solid battery stack 20 during charging and discharging.

固体電池積層体２０は表裏面を正電極プレート３０及び負電極プレート４０で覆われ、外周を樹脂筐体５０で覆われるので、外気から遮断され、使用中の水分や異物による劣化を防ぐことが可能である。また正電極プレート３０及び負電極プレート４０に厚みを持たせることで、機械的な外力が加わっても固体電池積層体２０にダメージが入るのを防ぐことができ、安全性を向上する効果が得られる。 The solid battery stack 20 is covered with the positive electrode plate 30 and the negative electrode plate 40 on the front and back surfaces, and is covered with the resin housing 50 on the outer periphery, so that it is shielded from the outside air and can be prevented from being deteriorated by moisture or foreign matter during use. It is possible. In addition, by making the positive electrode plate 30 and the negative electrode plate 40 thick, it is possible to prevent the solid battery stack 20 from being damaged even if a mechanical external force is applied, and an effect of improving safety can be obtained. be done.

モールド金型に樹脂を注入する際、正極２２や負極２４が固体電解質２６より大きく、固体電解質２６の外周にはみ出していると、注入された樹脂により変形し正極２２と負極２４が近接したり接触したりしてショート不良や信頼度低下につながるため、正極２２や負極２４は固体電解質２６より小さく形成する。 When the resin is injected into the molding die, if the positive electrode 22 or the negative electrode 24 is larger than the solid electrolyte 26 and protrudes outside the solid electrolyte 26, the injected resin deforms the positive electrode 22 and the negative electrode 24 so that the positive electrode 22 and the negative electrode 24 approach or contact each other. The positive electrode 22 and the negative electrode 24 are formed smaller than the solid electrolyte 26, because this leads to a short circuit and a decrease in reliability.

図３は、本発明の一実施形態によるモジュール構造を概略的に示す図である。
図３を参照すると、本発明の一実施形態によるモジュール構造１０は、図１に示す全固体電池の筐体構造１を複数個直列に接続した形態を有する。全固体電池の筐体構造１は略直方体であるが、隣接する全固体電池の筐体構造１の一方の露出する正電極プレート３０が、他方の全固体電池の筐体構造１の露出する負電極プレートと隣接するように直列に配列される。 FIG. 3 is a schematic diagram of a module structure according to an embodiment of the present invention.
Referring to FIG. 3, a module structure 10 according to an embodiment of the present invention has a form in which a plurality of casing structures 1 of all-solid-state batteries shown in FIG. 1 are connected in series. The case structure 1 of the all-solid-state battery has a substantially rectangular parallelepiped shape, but the exposed positive electrode plate 30 of one of the adjacent case structures 1 of the all-solid-state battery is the exposed negative electrode plate 30 of the other case structure 1 of the all-solid-state battery. The electrode plates are arranged in series adjacent to each other.

図３では６つの全固体電池の筐体構造１が直列に配列された構造を示すが、上記のように接続することで第１番目の全固体電池の筐体構造１の正電極プレート３０がモジュール構造１０の正電極となり、第６番目の負電極プレート４０がモジュール構造１０の負電極となる。尚モジュール構造１０が備える全固体電池の筐体構造１の数は６に限ることはなく、６より多くても少なくてもよい。積層する数によらず第１番目の全固体電池の筐体構造１の正電極プレート３０がモジュール構造１０の正電極となり、最後の全固体電池の筐体構造１の負電極プレート４０がモジュール構造１０の負電極となる。 FIG. 3 shows a structure in which six all-solid-state battery housing structures 1 are arranged in series. By connecting as described above, the positive electrode plate 30 of the first all-solid-state battery housing structure 1 The sixth negative electrode plate 40 serves as the positive electrode of the module structure 10 and the negative electrode of the module structure 10 . The number of casing structures 1 for all-solid-state batteries included in the module structure 10 is not limited to six, and may be more or less than six. Regardless of the number of stacks, the positive electrode plate 30 of the first all-solid-state battery housing structure 1 becomes the positive electrode of the module structure 10, and the last all-solid-state battery housing structure 1 of the negative electrode plate 40 becomes the module structure. 10 negative electrodes.

このように本発明による全固体電池の筐体構造１は、従来の全固体電池のように外部端子としてのタブが固体電池積層体２０から突出することがないので、複数の全固体電池の筐体構造１同士を接続するための接続エリアを別に設ける必要がなく、スペース効率の高いモジュール構造を実現することが可能である。 As described above, in the case structure 1 of the all-solid-state battery according to the present invention, tabs serving as external terminals do not protrude from the solid-state battery stack 20 unlike conventional all-solid-state batteries. It is not necessary to separately provide a connection area for connecting the body structures 1, and it is possible to realize a module structure with high space efficiency.

図４は図３に示すモジュール構造の内部構造を水平断面により概略的に示す図である。
前述のように樹脂筐体５０は正電極プレート３０及び負電極プレート４０の電極面より高く突出しないため単純に直列に配列することで電気的に直列接続されたモジュール構造を実現することができるが、正電極プレート３０及び負電極プレート４０の電極面に微小な凹凸や傾きがあると、正電極プレート３０と負電極プレート４０との間の接触抵抗が高くなってしまう恐れがある。 FIG. 4 is a diagram schematically showing the internal structure of the module structure shown in FIG. 3 in horizontal section.
As described above, since the resin casing 50 does not protrude higher than the electrode surfaces of the positive electrode plate 30 and the negative electrode plate 40, it is possible to realize an electrically series-connected module structure by simply arranging them in series. If the electrode surfaces of the positive electrode plate 30 and the negative electrode plate 40 have minute irregularities or inclinations, the contact resistance between the positive electrode plate 30 and the negative electrode plate 40 may increase.

そこで図４に示すモジュール構造では、隣接する全固体電池の筐体構造１の対向する正電極プレート３０と負電極プレート４０とは導電性材料６０を挟んで互いに接続される。ここで導電性材料６０は柔軟性を有する導電性板状部材又は導電性フィルム材、或は導電性のペースト材である。こうした柔軟性を有する導電性材料は一般に導電性の微小粒子が高密度に分散されており、圧力が加わって導電性材料が変形すると、中の微小粒子同士が接触し電気や熱を伝えるように構成されている。導電性材料６０はこうした導電性の微小粒子応用したものでもよいし、材料自体が導電性と変形性を有するものでもよい。 Therefore, in the module structure shown in FIG. 4, the positive electrode plate 30 and the negative electrode plate 40 facing each other in the casing structure 1 of the adjacent all-solid-state battery are connected to each other with the conductive material 60 interposed therebetween. Here, the conductive material 60 is a flexible conductive plate member, a conductive film material, or a conductive paste material. Conductive materials with such flexibility generally have conductive microparticles dispersed at a high density. It is configured. The conductive material 60 may be applied to such conductive fine particles, or the material itself may have conductivity and deformability.

このように柔軟性を有する導電性板状部材又は導電性フィルム材、或は導電性のペースト材を挟んで対向する正電極プレート３０と負電極プレート４０を互いに近接する方向に押し付けると、電極面に微小な凹凸や傾きがあっても柔軟性を有する導電性板状部材又は導電性フィルム材、或は導電性のペースト材が変形してこれを吸収するため、正電極プレート３０と負電極プレート４０との間の接触抵抗が高くなるのを防止することができる。 When the positive electrode plate 30 and the negative electrode plate 40 facing each other with a flexible conductive plate member, conductive film material, or conductive paste material sandwiched therebetween are pressed in the direction of approaching each other, the electrode surfaces The positive electrode plate 30 and negative electrode plate 40 can be prevented from increasing.

図５は、本発明の一実施形態によるモジュール構造の締結方法を概略的に示す図であり、図６は図５に示すモジュール構造の内部構造を水平断面により概略的に示す図である。
複数の全固体電池の筐体構造１を直列に接続してモジュール構造１０を形成するためには、接触抵抗の観点から隣接する全固体電池の筐体構造１を互いに押し付けるようにして固定することが望ましい。図５、６はこのための締結方法の一実施形態を示す。 FIG. 5 is a diagram schematically showing a fastening method of a module structure according to an embodiment of the present invention, and FIG. 6 is a diagram schematically showing the internal structure of the module structure shown in FIG. 5 in horizontal section.
In order to form a module structure 10 by connecting a plurality of all-solid-state battery casing structures 1 in series, adjacent all-solid-state battery casing structures 1 must be pressed against each other and fixed from the viewpoint of contact resistance. is desirable. Figures 5 and 6 show one embodiment of a fastening method for this purpose.

図５、６を参照すると、複数の全固体電池の筐体構造１を直列に配列した配列方向に沿って側方に一対の締結体７０が設けられ、複数の全固体電池の筐体構造１のそれぞれは締結ボルト７１によって締結体７０に固定されている。締結体７０は下方にＬ字状に折れ曲がり、取付け用のボルト穴を有する脚部を備えており、モジュール構造１０を使用する装置や車両の筐体に取り付けられるようになっている。 5 and 6, a pair of fasteners 70 are provided laterally along the direction in which the plurality of all-solid-state battery housing structures 1 are arranged in series, and the plurality of all-solid-state battery housing structures 1 are arranged sideways. are fixed to the fastening body 70 by fastening bolts 71 . The fastener 70 is bent downward into an L-shape and has legs with bolt holes for attachment, and is adapted to be attached to the housing of the device or vehicle that uses the module structure 10 .

図５、６に示すモジュール構造１０は、始めに第１番目の全固体電池の筐体構造１と一対の締結体７０とを締結ボルト７１によって固定した後、第２番目の全固体電池の筐体構造１を第１番目の全固体電池の筐体構造１に押し付けながら締結ボルト７１によって固定するというように順次全固体電池の筐体構造１を押し付けながら固定していくことで、全体として接触抵抗の上昇を防止したモジュール構造１０を形成することができる。このとき図４で示したような導電性材料６０を挟みこんで接続するようにしてもよい。また締結体７０の締結ボルト７１を貫通させるボルト穴は長穴として全固体電池の筐体構造１の取り付け位置を調整可能とするように構成してもよい。 5 and 6, the module structure 10 shown in FIGS. The body structure 1 is fixed by the fastening bolt 71 while being pressed against the housing structure 1 of the first all-solid-state battery. A module structure 10 that prevents an increase in resistance can be formed. At this time, a conductive material 60 as shown in FIG. 4 may be sandwiched for connection. Further, the bolt holes through which the fastening bolts 71 of the fastening body 70 pass may be formed as long holes so that the mounting position of the housing structure 1 of the all-solid-state battery can be adjusted.

尚、図６に示すモジュール構造１０に使用する全固体電池の筐体構造１は、図１に示すような略直方体形状のものとは少し形状が異なり、締結ボルト７１を締結するための突起状のねじ取付け部を有する。
他の実施形態では、締結ボルト７１の締結される部分の固体電池積層体２０に切り欠き部を設け、切り欠き部の中に納まるようにねじ取付け部を設けることで側面に突起が生じないような形状としてもよい。
図５、６に示す締結体７０の形状やこれを用いた締結方法は一つの実施形態であって、複数の全固体電池の筐体構造１が直列に密接された状態で保持できればこの締結方法には限らない。 The housing structure 1 of the all-solid-state battery used in the module structure 10 shown in FIG. has a screw mount.
In another embodiment, a notch is provided in the solid battery stack 20 at the portion to which the fastening bolt 71 is fastened, and a screw mounting portion is provided so as to fit in the notch so as not to generate a protrusion on the side surface. shape.
The shape of the fastening body 70 shown in FIGS. 5 and 6 and the fastening method using the fastening body 70 are one embodiment. is not limited to

以上、本発明の実施形態について図面を参照しながら詳細に説明したが、本発明は、上述の実施形態に限定されるものではなく、本発明の技術的範囲から逸脱しない範囲内で多様に変更することが可能である。 Although the embodiments of the present invention have been described in detail with reference to the drawings, the present invention is not limited to the above-described embodiments, and can be modified in various ways without departing from the technical scope of the present invention. It is possible to

１ 全固体電池の筐体構造
１０ モジュール構造
２０ 固体電池積層体
２１ 集電体
２２ 正極
２３ 正極電極
２４ 負極
２５ 負極電極
２６ 固体電解質
２７ バイポーラ電極
３０ 正電極プレート
４０ 負電極プレート
５０ 樹脂筐体
６０ 導電性材料
７０ 締結体
７１ 締結ボルト 1 Case Structure of All Solid Battery 10 Module Structure 20 Solid Battery Stack 21 Current Collector 22 Positive Electrode 23 Positive Electrode 24 Negative Electrode 25 Negative Electrode 26 Solid Electrolyte 27 Bipolar Electrode 30 Positive Electrode Plate 40 Negative Electrode Plate 50 Resin Case 60 Conductivity elastic material 70 fastening body 71 fastening bolt

Claims (1)

全固体電池の筐体構造を電気的に複数接続するモジュール構造であって、
前記全固体電池の筐体構造は、
集電体の片面に正極を形成した正極電極と、正極電極と対向し集電体の正極と対向する面に負極を形成した負極電極と、正極電極と負極電極との間に位置する複数の固体電解質と、隣接する複数の固体電解質の間にそれぞれ位置して集電体の片面に正極を形成し正極と反対側の面に負極を形成した複数のバイポーラ電極とを備える固体電池積層体と、
前記正極電極に隣接して配置された正電極プレートと、
前記負極電極に隣接して配置された負電極プレートと、
前記固体電池積層体、前記正電極プレート、及び前記負電極プレートの外周部を覆い、前記正電極プレート、及び前記負電極プレートの電極面が露出するように一体化する樹脂筐体と、を有し、
前記樹脂筐体は樹脂成型金型内で前記正電極プレートと、前記負電極プレートとを前記固体電池積層体に押し付ける加圧状態で注入されて固化されることで加圧状態を保ちつつ前記固体電池積層体を封止し、
前記複数の全固体電池の筐体構造は露出する正電極プレートが、他の全固体電池の筐体構造の露出する負電極プレートと隣接するように直列に配列され、
前記対向する正電極プレートと負電極プレートとは導電性材料を挟んで互いに接続され、
前記導電性材料は柔軟性を有する導電性板状部材又は導電性フィルム材、或は導電性のペースト材であることを特徴とするモジュール構造。


A module structure that electrically connects a plurality of housing structures of all-solid-state batteries,
The housing structure of the all-solid-state battery is
A positive electrode having a positive electrode formed on one side of a current collector, a negative electrode facing the positive electrode and having a negative electrode formed on a side of the current collector facing the positive electrode, and a plurality of electrodes positioned between the positive electrode and the negative electrode. A solid battery stack comprising a solid electrolyte and a plurality of bipolar electrodes positioned between a plurality of adjacent solid electrolytes, each having a positive electrode formed on one side of a current collector and a negative electrode formed on the opposite side of the positive electrode. ,
a positive electrode plate positioned adjacent to the positive electrode;
a negative electrode plate positioned adjacent to the negative electrode;
a resin casing that covers outer peripheral portions of the solid battery stack, the positive electrode plate, and the negative electrode plate, and integrates the positive electrode plate and the negative electrode plate so that electrode surfaces of the positive electrode plate and the negative electrode plate are exposed; death,
The resin casing is injected in a resin mold in a pressurized state that presses the positive electrode plate and the negative electrode plate against the solid battery stack and is solidified, thereby maintaining the pressurized state and solidifying the solid state. sealing the battery stack,
the plurality of all-solid-state battery housing structures are arranged in series such that exposed positive electrode plates are adjacent to exposed negative electrode plates of other all-solid-state battery housing structures ;
The positive electrode plate and the negative electrode plate facing each other are connected to each other with a conductive material interposed therebetween,
A module structure, wherein the conductive material is a flexible conductive plate member, a conductive film material, or a conductive paste material.


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