JP5487743B2 - Thin battery and manufacturing method thereof - Google Patents

Thin battery and manufacturing method thereof Download PDF

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JP5487743B2
JP5487743B2 JP2009140751A JP2009140751A JP5487743B2 JP 5487743 B2 JP5487743 B2 JP 5487743B2 JP 2009140751 A JP2009140751 A JP 2009140751A JP 2009140751 A JP2009140751 A JP 2009140751A JP 5487743 B2 JP5487743 B2 JP 5487743B2
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thin battery
tube
battery
conductor portion
internal space
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JP2010287451A (en
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紀之 松風
隆行 平尾
浄 一瀬
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Nissan Motor Co Ltd
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    • 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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  • Gas Exhaust Devices For Batteries (AREA)
  • Filling, Topping-Up Batteries (AREA)
  • Secondary Cells (AREA)
  • Connection Of Batteries Or Terminals (AREA)
  • Sealing Battery Cases Or Jackets (AREA)

Description

本発明は、薄型電池及びその製造方法に関するものである。   The present invention relates to a thin battery and a manufacturing method thereof.

缶状のリチウム二次電池において、缶内部に向けて膨らませて形成された凹部の注液口から電解液を注入したのち凹部内に金属球を装填し、次いで初充電を行うとともに初充電により発生したガスを注液口から排出し、最後に金属球を注液口に溶接するものが知られている（特許文献１）。 In a can-type lithium secondary battery, an electrolytic solution is injected from the injection port of a recess formed by inflating into the inside of the can, and then a metal ball is loaded into the recess, and then the first charge and the first charge are generated. It is known that the discharged gas is discharged from the injection port and finally a metal ball is welded to the injection port (Patent Document 1).

特許第３１７４２８９号公報Japanese Patent No. 3174289

ところで、薄型電池においても、電解液の注入、初充電により発生したガスの排出および電圧検出といった処理が必要とされるが、薄型電池に上記従来技術の構造を適用すると、不必要に厚くなり延いては電池の占有体積が増加するという問題がある。 By the way, even in a thin battery, treatments such as injection of electrolyte, discharge of gas generated by initial charging, and voltage detection are required. However, if the structure of the above prior art is applied to a thin battery, the thickness becomes unnecessarily thick. In this case, the occupied volume of the battery increases.

本発明が解決しようとする課題は、占有体積を増加させることなく電解液の注入、ガスの排出及び電圧の検出の各処理が実行できる薄型電池及びその製造方法を提供することである。   The problem to be solved by the present invention is to provide a thin battery and a method for manufacturing the same that can perform the processes of injecting electrolyte, discharging gas, and detecting voltage without increasing the occupied volume.

本発明は、絶縁性外筒部に被覆された封止可能な第１導体部および第２導体部を有するチューブを、電池内外部を封止するシール部を貫通するように設けることによって上記課題を解決する。 The present invention provides the above-described problem by providing a tube having a sealable first conductor portion and a second conductor portion covered with an insulating outer cylinder portion so as to penetrate a seal portion that seals the inside and outside of the battery. To solve.

本発明では、電池の内外部を封止するシール部にチューブを設け、当該チューブを介して電解液を注入したのちチューブの電池外部側の第２導体部を封止する。ついで、初充電をしたのちに電池内部のガスを排出する際は電池外部側の第２導体部を切除し、ガス排出後はチューブの電池内部側の第１導体部を封止する。これにより、電池の占有体積を増加させることなく電解液の注入とガス排出を行うことができる。   In the present invention, a tube is provided in a seal portion that seals the inside and outside of the battery, and after the electrolyte is injected through the tube, the second conductor portion on the battery outside of the tube is sealed. Next, when the gas inside the battery is discharged after the initial charge, the second conductor part on the battery outer side is cut off, and after the gas discharge, the first conductor part on the battery inner side of the tube is sealed. As a result, the electrolyte can be injected and the gas discharged without increasing the occupied volume of the battery.

一方、発電要素に接続された第１導体部と電池外部の第２導体部は導通しているので、電池外部の第２導体部を介して発電要素の電圧検出を行うことができる。   On the other hand, since the first conductor portion connected to the power generation element is electrically connected to the second conductor portion outside the battery, the voltage of the power generation element can be detected via the second conductor portion outside the battery.

本発明の一実施の形態を適用したバイポーラ薄型電池を示す断面図である。It is sectional drawing which shows the bipolar thin battery to which one embodiment of this invention is applied. 図１のバイポーラ薄型電池を示す外観斜視図である。It is an external appearance perspective view which shows the bipolar thin battery of FIG. 図１のチューブを示す斜視図である。It is a perspective view which shows the tube of FIG. 図１のチューブの装着状態を示す拡大断面図である。It is an expanded sectional view which shows the mounting state of the tube of FIG. 図１のバイポーラ薄型電池の製造方法を示す断面図（その１）である。FIG. 3 is a sectional view (No. 1) showing a method for manufacturing the bipolar thin battery of FIG. 図１のバイポーラ薄型電池の製造方法を示す断面図（その２）である。FIG. 4 is a sectional view (No. 2) showing the method for manufacturing the bipolar thin battery of FIG. 図１のバイポーラ薄型電池の製造方法を示す断面図（その３）である。FIG. 4 is a sectional view (No. 3) showing the method for manufacturing the bipolar thin battery of FIG. 図１のバイポーラ薄型電池の製造方法を示す断面図（その４）である。FIG. 6 is a sectional view (No. 4) showing the method for manufacturing the bipolar thin battery of FIG. 本発明の他の実施の形態を適用したバイポーラ薄型電池を示す平面図である。It is a top view which shows the bipolar thin battery to which other embodiment of this invention is applied.

以下、本発明の実施形態を図面に基づいて説明する。   Hereinafter, embodiments of the present invention will be described with reference to the drawings.

図１は、本発明の一実施の形態を適用したバイポーラ薄型電池を示す主要断面図、図２はその外観斜視図である。なお、図１に示す各部材は、薄型電池の構造をより理解しやすくするために特に厚さ寸法を誇張して示すが、実際の厚さ等の寸法は後述するとおりである。また、本例のバイポーラ電池はリチウムイオン二次電池として説明するが、二次電池の種類には特に限定されず他の二次電池にも適用することができる。   FIG. 1 is a main sectional view showing a bipolar thin battery to which an embodiment of the present invention is applied, and FIG. 2 is an external perspective view thereof. In addition, although each member shown in FIG. 1 exaggerates especially the thickness dimension in order to make the structure of a thin battery easier to understand, the dimensions such as the actual thickness are as described later. In addition, although the bipolar battery of this example will be described as a lithium ion secondary battery, the type of the secondary battery is not particularly limited, and can be applied to other secondary batteries.

図１に示すように、本例のバイポーラ薄型電池１（以下、単に電池１とも言う）は、正極１３２、負極１３３および集電体１３１を有するバイポーラ電極１３と、セパレータ１３４および電解液１３５を含む電解質層１３６と、第１シール部１４１および第２シール部１４２を含むシール部１４と、これらを外包する上部外装部材１５１及び下部外装部材１５２を含む外装部材１５と、を備える。   As shown in FIG. 1, the bipolar thin battery 1 (hereinafter also simply referred to as the battery 1) of this example includes a bipolar electrode 13 having a positive electrode 132, a negative electrode 133, and a current collector 131, a separator 134, and an electrolyte solution 135. An electrolyte layer 136, a seal portion 14 including a first seal portion 141 and a second seal portion 142, and an exterior member 15 including an upper exterior member 151 and a lower exterior member 152 that enclose them are provided.

発電要素の一単位となるバイポーラ電極１３は、集電体１３１の一方の主面に正極１３２が形成され、他方の主面に負極１３３が形成されてなる。   The bipolar electrode 13, which is a unit of the power generation element, has a positive electrode 132 formed on one main surface of the current collector 131 and a negative electrode 133 formed on the other main surface.

集電体１３１は、ステンレススチール箔、アルミニウム箔、ニッケルとアルミニウムのクラッド材、銅とアルミニウムのクラッド材、あるいはこれらの金属の組み合わせのめっき材などの導電性材料から構成されている。   The current collector 131 is made of a conductive material such as a stainless steel foil, an aluminum foil, a clad material of nickel and aluminum, a clad material of copper and aluminum, or a plating material of a combination of these metals.

正極１３２の正極活物質は、容量および出力特性の観点から、マンガン酸リチウムＬｉＭｎ２Ｏ４、コバルト酸リチウムその他のリチウム−遷移金属複合酸化物などの材料から構成されている。一方、負極１３３の負極活物質は、容量および出力特性の観点から、ハードカーボン（難黒鉛化炭素材料）、黒鉛系炭素材料、リチウム−遷移金属複合酸化物などの材料から構成されている。 The positive electrode active material of the positive electrode 132 is made of a material such as lithium manganate LiMn 2 O 4 , lithium cobaltate, or other lithium-transition metal composite oxide from the viewpoint of capacity and output characteristics. On the other hand, the negative electrode active material of the negative electrode 133 is made of a material such as hard carbon (non-graphitizable carbon material), a graphite-based carbon material, or a lithium-transition metal composite oxide from the viewpoint of capacity and output characteristics.

これら正極１３２および負極１３３の厚さは、電池の使用目的、例えば出力重視の電池か否か、エネルギー重視の電池か否かといった目的や、イオン伝導性を考慮して適宜設定される。   The thicknesses of the positive electrode 132 and the negative electrode 133 are appropriately set in consideration of the purpose of use of the battery, for example, whether the battery is output-oriented or energy-oriented, and ion conductivity.

第１シール部１４１は、集電体１３１の一方の主面に、正極１３２を取り囲むように配置されている。また第２シール部１４２は、集電体１３１の他方の面であって第１シール部１４１の位置と同じ背面位置に、負極１３３を取り囲むように配置されている。   The first seal portion 141 is disposed on one main surface of the current collector 131 so as to surround the positive electrode 132. The second seal portion 142 is disposed on the other surface of the current collector 131 and at the same back surface position as the first seal portion 141 so as to surround the negative electrode 133.

これら第１シール部１４１および第２シール部１４２を構成するシール材は、一液硬化性エポキシ樹脂その他の熱硬化型樹脂、ポリプロピレン、ポリエチレンその他の熱可塑型樹脂などの絶縁性材料から構成されている。シール部１４を構成する材料は、使用環境下において良好なシール効果を発揮するものを電池の用途に応じて適宜選択することが好ましい。   The sealing material constituting the first seal part 141 and the second seal part 142 is made of an insulating material such as a one-part curable epoxy resin or other thermosetting resin, polypropylene, polyethylene or other thermoplastic resin. Yes. It is preferable that the material constituting the seal portion 14 is appropriately selected according to the intended use of the battery so as to exhibit a good sealing effect in the use environment.

セパレータ１３４は、隣接する２つの集電体１３１，１３１の間であって、一方の主面が正極１３２および第１シール部１４１を覆い、他方の主面が負極１３３および第２シール部１４２を覆うように配置されている。   The separator 134 is between two adjacent current collectors 131, 131, one main surface covering the positive electrode 132 and the first seal portion 141, and the other main surface covering the negative electrode 133 and the second seal portion 142. It is arranged to cover.

セパレータ１３４は、正極と負極を区分けする通気性を有するポーラス状部材であって、当該セパレータ１３４内にゲルポリマー系電解質を含浸させる。このセパレータ１３４は、正極１３２と負極１３３との直接的な接触を阻止する絶縁体であるが、セパレータ１３４に形成された多数の孔の内部に電解質が浸透することで、イオン及び電流が流れることになる。   The separator 134 is a porous member having air permeability that separates the positive electrode and the negative electrode, and the separator 134 is impregnated with a gel polymer electrolyte. The separator 134 is an insulator that prevents direct contact between the positive electrode 132 and the negative electrode 133, but ions and current flow when the electrolyte permeates into a large number of holes formed in the separator 134. become.

また、セパレータ１３４、集電体１３１および第１シール部１４１又は第２シール部１４２で画成された空間には、セパレータ１３４と正極１３２または負極１３３との間でイオンを伝導する電解液（電解質）１３５が封入されている。これら電解質を含浸したセパレータ１３４および電解液１３５を併せて電解質層１３６と称する。   Further, in a space defined by the separator 134, the current collector 131 and the first seal portion 141 or the second seal portion 142, an electrolyte solution (electrolyte) that conducts ions between the separator 134 and the positive electrode 132 or the negative electrode 133 is used. ) 135 is enclosed. The separator 134 impregnated with the electrolyte and the electrolytic solution 135 are collectively referred to as an electrolyte layer 136.

上述したセパレータ１３４の通気性（多孔性）を有する素材として、ポリエチレンＰＥ、ポリプロピレンＰＰその他のポリオレフィン系樹脂、ＰＰ／ＰＥ／ＰＰの３層構造をした積層体、ポリアミド、ポリイミド、アラミド、不織布などを使用することができる。不織布としては、例えば、綿、レーヨン、アセテート、ナイロン、ポリエステルを挙げることができる。   As the material having the air permeability (porosity) of the separator 134 described above, polyethylene PE, polypropylene PP and other polyolefin resins, laminates having a three-layer structure of PP / PE / PP, polyamide, polyimide, aramid, non-woven fabric, etc. Can be used. Examples of the non-woven fabric include cotton, rayon, acetate, nylon, and polyester.

電解質の電解液は、プロピレンカーボネートＰＣおよびエチレンカーボネートＥＣからなる有機溶媒、支持塩としてのリチウム塩ＬｉＰＦ６を含んでいる。有機溶媒は、ＰＣおよびＥＣに特に限定されず、例えば、その他の環状カーボネート類、ジメチルカーボネート等の鎖状カーボネート類、テトラヒドロフラン等のエーテル類を使用することができる。またリチウム塩は、ＬｉＰＦ６その他の無機酸陰イオン塩、ＬｉＣＦ３ＳＯ３等の有機酸陰イオン塩を使用することができる。 The electrolytic solution of the electrolyte contains an organic solvent composed of propylene carbonate PC and ethylene carbonate EC, and a lithium salt LiPF 6 as a supporting salt. The organic solvent is not particularly limited to PC and EC, and for example, other cyclic carbonates, chain carbonates such as dimethyl carbonate, and ethers such as tetrahydrofuran can be used. As the lithium salt, organic acid anion salts such as LiPF 6 and other inorganic acid anion salts and LiCF 3 SO 3 can be used.

電解質のホストポリマーは、ＨＦＰ（ヘキサフルオロプロピレン）コポリマーを１０％含むＰＶＤＦ−ＨＦＰ（ポリフッ化ビニリデンとヘキサフルオロプロピレンの共重合体）その他のリチウムイオン伝導性を持たない高分子や、イオン伝導性を有する高分子（固体高分子電解質）を使用することができる。リチウムイオン伝導性を持たない高分子としては、ポリアクリロニトリルＰＡＮやポリメチルメタクリレートＰＭＭＡを挙げることができる。また、イオン伝導性を有する高分子としては、ポリエチレンオキシドＰＥＯやポリプロピレンオキシドＰＰＯを挙げることができる。   The electrolyte host polymer is PVDF-HFP (polyvinylidene fluoride-hexafluoropropylene copolymer) containing 10% HFP (hexafluoropropylene) copolymer, other polymers that do not have lithium ion conductivity, and ion conductivity. The polymer (solid polymer electrolyte) which has can be used. Examples of the polymer having no lithium ion conductivity include polyacrylonitrile PAN and polymethyl methacrylate PMMA. Examples of the polymer having ion conductivity include polyethylene oxide PEO and polypropylene oxide PPO.

図２に示すバイポーラ電池１は、図１に示すように複数のバイポーラ電極１３（発電要素）を積層体１３７とした形態で、外部からの衝撃や環境劣化を防止するための外装部材１５に収容されている。バイポーラ電極１３の積層体１３７の最外層（最上位および最下位）には、正極端子プレート１１と負極端子プレート１２がそれぞれ配置される。なお、これら端子プレート１１，１２の更に外側に補強板を配置することもできる。   A bipolar battery 1 shown in FIG. 2 is housed in an exterior member 15 for preventing impact from the outside and environmental degradation in the form of a laminated body 137 having a plurality of bipolar electrodes 13 (power generation elements) as shown in FIG. Has been. The positive electrode terminal plate 11 and the negative electrode terminal plate 12 are disposed on the outermost layers (the uppermost layer and the lowermost layer) of the stacked body 137 of the bipolar electrode 13. In addition, a reinforcing plate can be disposed further outside the terminal plates 11 and 12.

正極端子プレート１１および負極端子プレート１２は、アルミニウム、銅、チタン、ニッケル、ステンレス、これらの合金などの高導電性部材からなり、少なくとも積層体１３７の最外層の電極投影面の全てを覆うように構成されている。これにより、最外層の電流取り出し部の抵抗が低くなり、面方向の電流取り出しにおける低抵抗化を図ることで、電池の高出力化が可能になる。   The positive electrode terminal plate 11 and the negative electrode terminal plate 12 are made of a highly conductive member such as aluminum, copper, titanium, nickel, stainless steel, or an alloy thereof so as to cover at least all the electrode projection surfaces of the outermost layer of the laminate 137. It is configured. As a result, the resistance of the current extraction portion in the outermost layer is lowered, and the reduction in resistance in the current extraction in the surface direction makes it possible to increase the output of the battery.

正極端子プレート１１および負極端子プレート１２は、それぞれ外装部材１５の外部に引き出され、積層体１３７から電流を引き出すための電極タブとして機能する。なお、独立した別体の電極タブを、直接的あるいはリードを利用して端子プレート１１，１２と接続することで、積層体１３７から電流を引き出すこともできる。また、積層体１３７の最外層に位置する集電体１３１によって、端子プレート１１，１２を構成してもよい。   The positive electrode terminal plate 11 and the negative electrode terminal plate 12 are each drawn out of the exterior member 15 and function as electrode tabs for drawing current from the stacked body 137. In addition, an electric current can also be drawn from the laminated body 137 by connecting an independent separate electrode tab to the terminal plates 11 and 12 directly or using a lead. Further, the terminal plates 11 and 12 may be configured by the current collector 131 located in the outermost layer of the stacked body 137.

外装部材１５は、軽量化および熱伝導性の観点から、アルミニウム、ステンレス、ニッケル、銅などの金属（合金を含む）をポリプロピレンフィルム等の絶縁体で被覆した高分子−金属複合ラミネートフィルムなどのシート材からなり、その外周部の一部または全部を熱融着することで形成される。   The exterior member 15 is a sheet such as a polymer-metal composite laminate film in which a metal (including an alloy) such as aluminum, stainless steel, nickel, or copper is covered with an insulator such as a polypropylene film from the viewpoint of weight reduction and thermal conductivity. It is made of a material and is formed by heat-sealing part or all of the outer periphery.

なお、図２に示す電池１を単独で使用することも可能であるが、複数の電池１を直列および／または並列に接続し、組電池の形態で使用することもできる。組電池を構成する際に、直列および並列の組み合わせを適宜設定することで、容量および電圧を自由に調整することができる。電池１の電極タブ（端子プレート１１，１２）の接続は、超音波溶接、熱溶接、レーザー溶接、リベット、かしめ、電子ビームなどの諸方法により行うことができる。   The battery 1 shown in FIG. 2 can be used alone, but a plurality of batteries 1 can be connected in series and / or in parallel to be used in the form of an assembled battery. When configuring the assembled battery, the capacity and voltage can be freely adjusted by appropriately setting the combination of series and parallel. The electrode tabs (terminal plates 11 and 12) of the battery 1 can be connected by various methods such as ultrasonic welding, heat welding, laser welding, rivets, caulking, and electron beam.

こうした組電池や組電池をさらに組み合わせた組電池モジュールは、大出力を確保し得るため、電気自動車、ハイブリッド自動車、電車などの各種車両のモータ駆動用電源として利用することができる。組電池や組電池モジュールは、それを構成する電池１ごと又は組電池ごとに、非常にきめ細かい充放電制御ができるため、１回の充電あたりの走行距離の延長や、車載電池としての寿命の長期化などの性能の向上を図ることが可能である。   Such an assembled battery or an assembled battery module obtained by further combining the assembled batteries can ensure a large output, and can be used as a power source for driving motors of various vehicles such as electric vehicles, hybrid vehicles, and trains. The assembled battery and the assembled battery module can perform very fine charge / discharge control for each battery 1 or each assembled battery constituting the assembled battery and the assembled battery module, so that the travel distance per charge can be extended and the life of the vehicle battery can be extended. It is possible to improve the performance, such as.

本例の電池１は、シール部１４（図１に示す例では第２シール部１４２）を貫通するチューブ２０をさらに備える。このチューブ２０の一端は、セパレータ１３４、集電体１３１および第２シール部１４２で画成された内部空間Ｓに臨み、他端は第２シール部１４２の外部空間に臨むように設けられている。   The battery 1 of this example further includes a tube 20 that penetrates the seal portion 14 (second seal portion 142 in the example shown in FIG. 1). One end of the tube 20 faces the internal space S defined by the separator 134, the current collector 131 and the second seal portion 142, and the other end faces the external space of the second seal portion 142. .

本例のチューブ２０の外観を図３に示し、バイポーラ電極１３に装着した状態を図４に示す。図４は、図１に示す３つのバイポーラ電極１３のうちのひとつのバイポーラ電極１３の要部を示す断面図である。   The external appearance of the tube 20 of this example is shown in FIG. 3, and the state attached to the bipolar electrode 13 is shown in FIG. FIG. 4 is a cross-sectional view showing the main part of one of the three bipolar electrodes 13 shown in FIG.

図３に示すように、本例のチューブ２０は、一端に設けられた第１導体部２０１と、他端に設けられた第２導体部２０２と、これら第１導体部２０１および第２導体部２０２を被覆する外筒部２０３と、を備える。   As shown in FIG. 3, the tube 20 of this example includes a first conductor portion 201 provided at one end, a second conductor portion 202 provided at the other end, and the first conductor portion 201 and the second conductor portion. And an outer cylinder portion 203 that covers 202.

第１導体部２０１は、後述する封止前には所定の開口面積を有するとともに封止後は当該開口を閉塞して所定の厚さを有する可撓性の材料から構成され、本例では軸方向に所定長を有する、銅、アルミニウム、これらの合金、導電性樹脂などの導体からなる筒状体で構成されている。この第１導体部２０１は、図４に示すように、セパレータ１３４、集電体１３１および第２シール部１４２で画成された内部空間Ｓに臨むように設けられる。   The first conductor portion 201 is made of a flexible material having a predetermined opening area before sealing, which will be described later, and having a predetermined thickness by closing the opening after sealing. It is comprised with the cylindrical body which consists of conductors, such as copper, aluminum, these alloys, and conductive resin, which has predetermined length in a direction. As shown in FIG. 4, the first conductor portion 201 is provided so as to face the internal space S defined by the separator 134, the current collector 131, and the second seal portion 142.

第２導体部２０２は、第１導体部２０１に接続されて軸方向に延在する接続部２０２Ａと、この接続部２０２Ａに接続され、封止前に所定の開口面積を有するとともに後述する初充電後に切除される封止切除部２０２Ｂとを有する。本例の第２導体部２０２は、板状の接続部２０２Ａと、軸方向に所定長を有する筒状の封止切除部２０２Ｂとを備え、上述した第１導体部２０１と同じように、銅、アルミニウム、これらの合金、導電性樹脂などの可撓性を有する導体から構成されている。この第２導体部２０２の封止切除部２０２Ｂは、第２シール部１４２の外部空間に臨むように設けられる。   The second conductor portion 202 is connected to the first conductor portion 201 and extends in the axial direction. The second conductor portion 202 is connected to the connection portion 202A, has a predetermined opening area before sealing, and has an initial charge described later. And a sealing excision part 202B to be excised later. The second conductor portion 202 of this example includes a plate-like connection portion 202A and a cylindrical sealing cutout portion 202B having a predetermined length in the axial direction, and, like the first conductor portion 201 described above, , Aluminum, alloys thereof, and conductive conductors. The sealing cut portion 202B of the second conductor portion 202 is provided so as to face the external space of the second seal portion 142.

なお、第１導体部２０１と第２導体部２０２は同じ材料で一体的に形成してもよく、また異なる材料で別々に形成したのち接合してもよい。   In addition, the 1st conductor part 201 and the 2nd conductor part 202 may be integrally formed with the same material, and after forming separately with a different material, you may join.

外筒部２０３は、ポリイミド樹脂などの絶縁体からなる所望長を有する筒体であって、先端から上記第１導体部２０１の一部が露出するように、第１導体部２０１と第２導体部２０２を外筒部２０３の先端から挿入することで、これら第１導体部２０１と第２導体部２０２を被覆する。外筒部２０３の外径は、バイポーラ電極１３の大きさに応じて適宜選択され、たとえば０．１ｍｍ〜３ｍｍである。外筒部２０３の他端（図３及び図４において左端）は、電解液の注入装置に装着される。   The outer cylinder part 203 is a cylinder having a desired length made of an insulator such as polyimide resin, and the first conductor part 201 and the second conductor are exposed so that a part of the first conductor part 201 is exposed from the tip. The first conductor portion 201 and the second conductor portion 202 are covered by inserting the portion 202 from the tip of the outer cylinder portion 203. The outer diameter of the outer cylinder part 203 is appropriately selected according to the size of the bipolar electrode 13 and is, for example, 0.1 mm to 3 mm. The other end (the left end in FIGS. 3 and 4) of the outer cylinder portion 203 is attached to an electrolytic solution injection device.

なお、外筒部２０３は断面円形にのみ限定されず、第１導体部２０１や封止切除部２０２Ｂとともに断面矩形とすることもできる。   The outer cylinder portion 203 is not limited to a circular cross section, and may be a rectangular cross section together with the first conductor portion 201 and the sealing cutout portion 202B.

このように構成されたチューブ２０は、図４に示すように一つのバイポーラ電極１３に１つ設けられ、図１に示す薄型電池１全体では３つ設けられている。そして、図４に示すようにチューブ２０は第２シール部１４２を貫通し、第１導体部２０２が集電体１３１に溶接または接着などにより接合されている。   As shown in FIG. 4, one tube 20 configured as described above is provided for one bipolar electrode 13, and three thin batteries 1 shown in FIG. 1 are provided as a whole. As shown in FIG. 4, the tube 20 passes through the second seal portion 142, and the first conductor portion 202 is joined to the current collector 131 by welding or adhesion.

これにより、薄型電池１全体として３つの集電体１３１それぞれにチューブ２０の第１導体部２０２が接続され、そのチューブ２０の他端である第２導体部２０２が外装部材１５の外まで導出されるので、各バイポーラ電極１３の電圧測定が可能となる。   Accordingly, the first conductor portion 202 of the tube 20 is connected to each of the three current collectors 131 as the thin battery 1 as a whole, and the second conductor portion 202 that is the other end of the tube 20 is led out of the exterior member 15. Therefore, voltage measurement of each bipolar electrode 13 becomes possible.

次に製法を説明する。   Next, the production method will be described.

図５Ａ〜図５Ｄは、図１に示すバイポーラ薄型電池１の製造方法を示す断面図であり、一つのバイポーラ電極１３の要部を示す図（図４に相当する断面図）である。   5A to 5D are cross-sectional views showing a method of manufacturing the bipolar thin battery 1 shown in FIG. 1, and are views (a cross-sectional view corresponding to FIG. 4) showing the main part of one bipolar electrode 13. FIG.

バイポーラ薄型電池１は、たとえば集電体１３１の両面に正極１３２および負極１３３を形成し、これにセパレータ１３４を積層したサブアッシユニットとしての集成体を形成したのち、これら複数の集成体をさらに積層して積層体を形成し、最後に積層体を外装ケースに収容することにより製造される。   In the bipolar thin battery 1, for example, a positive electrode 132 and a negative electrode 133 are formed on both surfaces of a current collector 131, and an assembly as a subassembly unit in which a separator 134 is stacked thereon is formed, and then the plurality of assemblies are further stacked. The laminate is formed, and finally the laminate is housed in an exterior case.

集電体１３１の両面に正極１３２および負極１３３を形成するには、スラリー状に調製された正極材料および負極材料をステンレススチール箔などからなる集電体１３１の両面のそれぞれに塗布し、真空オーブンなどにより乾燥する。   In order to form the positive electrode 132 and the negative electrode 133 on both surfaces of the current collector 131, the positive electrode material and the negative electrode material prepared in the form of slurry are applied to both surfaces of the current collector 131 made of stainless steel foil or the like, and a vacuum oven Dry by etc.

次いで、両面に正極１３２および負極１３３が形成された集電体１３１の外周に、正極１３２または負極１３３を取り囲むように１液硬化型エポキシ樹脂などのシール材を塗布し、これにセパレータ１３４を重ねる。これにより、集電体１３１の正極１３２が形成された主面の外周に第１シール部１４１が形成され、集電体１３１の負極１３３が形成された主面の外周に第２シール部１４２が形成される。なお、シール材を塗布したら自然乾燥または所定の温度に保持し、これを乾燥硬化させる。   Next, a sealing material such as a one-component curable epoxy resin is applied to the outer periphery of the current collector 131 having the positive electrode 132 and the negative electrode 133 formed on both sides so as to surround the positive electrode 132 or the negative electrode 133, and the separator 134 is stacked thereon. . Thus, the first seal portion 141 is formed on the outer periphery of the main surface of the current collector 131 where the positive electrode 132 is formed, and the second seal portion 142 is formed on the outer periphery of the main surface of the current collector 131 where the negative electrode 133 is formed. It is formed. When the sealing material is applied, it is naturally dried or kept at a predetermined temperature and dried and cured.

本例では、第２シール部１４２を構成するシール材を集電体１３１の外周に塗布する際に、図５Ａに示すように薄型電池１の１辺にチューブ２０を介装する。このとき、チューブ２０の第１導体部２０１と集電体１３１とを接合する。また、それぞれのチューブ２０は外装部材１５の外周部から外部へ導出するので、互いに干渉しないように平面視において少しずつずれた位置に設けられる。   In this example, when the sealing material constituting the second seal portion 142 is applied to the outer periphery of the current collector 131, the tube 20 is interposed on one side of the thin battery 1 as shown in FIG. 5A. At this time, the first conductor 201 of the tube 20 and the current collector 131 are joined. Moreover, since each tube 20 is derived | led-out from the outer peripheral part of the exterior member 15, it is provided in the position shifted | deviated little by little in planar view so that it may not mutually interfere.

この状態で、図５Ａに示すようにチューブ２０の左端から内部空間Ｓへ電解液１３５を注入する。このとき、第１導体部２０１および第２導体部２０２の封止切除部２０２Ｂは所定の開口面積を有するので、外筒部２０３によって内部空間Ｓへ電解液１３５を充填することができる。なお、本例ではチューブ２０を第２シール部１４２のみに貫通するように設け、第１シール部１４１には設けていないが、内部空間Ｓから注入された電解液はセパレータ１３４を介して対面する内部空間（第１シール部１４１に相当する空間）にも浸透することになる。   In this state, as shown in FIG. 5A, the electrolytic solution 135 is injected into the internal space S from the left end of the tube 20. At this time, since the sealing cut portion 202B of the first conductor portion 201 and the second conductor portion 202 has a predetermined opening area, the inner space S can be filled with the electrolyte solution 135 by the outer cylinder portion 203. In this example, the tube 20 is provided so as to penetrate only the second seal portion 142 and is not provided in the first seal portion 141, but the electrolyte injected from the internal space S faces through the separator 134. It also penetrates into the internal space (the space corresponding to the first seal portion 141).

各集成体（サブアッシユニット）に電解液を注入したら、図５Ｂに示すようにチューブ２０の封止切除部２０２Ｂを外筒部２０３とともに押し潰し、チューブ２０から電解液が漏洩しないように封止する。   After injecting the electrolyte into each assembly (sub-assembly unit), as shown in FIG. 5B, the sealing and cutting part 202B of the tube 20 is crushed together with the outer cylinder part 203 and sealed so that the electrolyte does not leak from the tube 20 To do.

チューブ２０の封止切除部２０２Ｂが封止された集成体をさらに複数積層して図１の実線で示す積層体を形成し、さらにこの積層体を外装部材１５にて封止する。   A plurality of assemblies in which the sealing cut portions 202B of the tubes 20 are sealed are further stacked to form a stacked body indicated by a solid line in FIG. 1, and the stacked body is further sealed with the exterior member 15.

なお、電解液の注入は集成体（サブアッシユニット）を形成したのちに行ってもよい。また、後述する初充電とガス抜きは積層体を外装部材１５にて封止する前に行ってもよい。   In addition, you may perform injection | pouring of electrolyte solution, after forming an assembly (sub assembly unit). In addition, initial charging and degassing described later may be performed before the laminate is sealed with the exterior member 15.

次いで、図５Ｂに示すようにチューブ２０の封止切除部２０２Ｂが封止された状態で、図１に示す正極端子プレート１１および負極端子プレート１２に電圧を印加し、初充電を実行する。これにより、薄型電池１の各バイポーラ電極１３に充電が行われるが、この充電反応によるガスが電池内部に発生する。   Next, as shown in FIG. 5B, in a state where the sealing cut portion 202B of the tube 20 is sealed, a voltage is applied to the positive terminal plate 11 and the negative terminal plate 12 shown in FIG. As a result, each bipolar electrode 13 of the thin battery 1 is charged, but gas due to this charging reaction is generated inside the battery.

初充電を終了したら、図５Ｃに示すようにチューブ２０の封止切除部２０２Ｂを切除し、再びチューブ２０によって内部空間Ｓと電池外部とを連通させる。そして、この状態で所定気圧に減圧した減圧室に電池１を入れ、電池内部に発生したガスを、チューブ２０を介して電池外部へ排出する。   When the initial charging is completed, as shown in FIG. 5C, the sealing cut portion 202 </ b> B of the tube 20 is cut, and the internal space S and the outside of the battery are communicated again by the tube 20. In this state, the battery 1 is placed in a decompression chamber decompressed to a predetermined pressure, and the gas generated inside the battery is discharged to the outside of the battery via the tube 20.

ガスの排出を終了したら、図５Ｄに示すように今度はチューブ２０の第１導体部２０１の左端を外筒部２０３とともに押し潰し、チューブ２０を封止する。これにより、チューブ２０から電解液が漏洩することを防止できる。第１導体部２０１を押し潰すには、たとえば外装部材１５の上から局部的な力を加えることで可撓性を有する第１導体部２０１を押し潰すことができる。   When the gas discharge is completed, as shown in FIG. 5D, the left end of the first conductor portion 201 of the tube 20 is now crushed together with the outer cylinder portion 203 to seal the tube 20. Thereby, it is possible to prevent the electrolytic solution from leaking from the tube 20. In order to crush the first conductor part 201, for example, the first conductor part 201 having flexibility can be crushed by applying a local force from above the exterior member 15.

このとき、チューブ２０の第１導体部２０１の右端、すなわち内部空間Ｓに望む部分を押し潰してもよいが、本例では開口させておく。これにより、薄型電池１を使用中に内部の圧力が上昇すると、当該第１導体部２０１の開口にガス圧が集中し、チューブ２０が安全弁として機能する。   At this time, the right end of the first conductor portion 201 of the tube 20, that is, a desired portion in the internal space S may be crushed, but in this example, it is opened. Thereby, when an internal pressure rises while using the thin battery 1, the gas pressure concentrates on the opening of the first conductor portion 201, and the tube 20 functions as a safety valve.

一方、第１導体部２０１の押し潰した部分は集電体１３１に重なるように接するので、電池１の外周部に積層方向の外力が作用すると、これを集電体１３１だけでなく第１導体部２０１の押し潰した部分でも受けることになる。したがって、集電体１３１への応力集中を緩和することができる。   On the other hand, since the crushed portion of the first conductor portion 201 is in contact with the current collector 131, when an external force in the stacking direction acts on the outer peripheral portion of the battery 1, not only the current collector 131 but also the first conductor Even the crushed part of the part 201 is received. Therefore, stress concentration on the current collector 131 can be reduced.

以上の工程により本例の薄型電池１が得られる（図１参照）が、チューブ２０の第２導体部２０２の接続部２０２Ａは第１導体部２０１を介して集電体１３１に電気的に接続されているので、この接続部２０２Ａに電圧検出端子を接続することで集電体１３１間の電圧を測定することができる。   Although the thin battery 1 of this example is obtained by the above steps (see FIG. 1), the connection portion 202A of the second conductor portion 202 of the tube 20 is electrically connected to the current collector 131 via the first conductor portion 201. Therefore, the voltage between the current collectors 131 can be measured by connecting a voltage detection terminal to the connecting portion 202A.

以上のとおり、本例の薄型電池１によれば、第２シール部１４２を貫通するようにチューブ２０を設けているので、薄型電池１の厚さ方向の寸法はそのままの寸法を維持することができ、占有体積は変わらない。その上で、当該チューブ２０により電解液の注入とガス抜きを行うことができる。   As described above, according to the thin battery 1 of this example, since the tube 20 is provided so as to penetrate the second seal portion 142, the thickness of the thin battery 1 can be maintained as it is. Yes, the occupied volume does not change. Then, the electrolyte solution can be injected and degassed by the tube 20.

また、薄型電池完成後においては、残った第１導体部２０１と第２導体部２０２とを用いて集電体１３１間の電圧、すなわちバイポーラ電極１３の電圧を測定することもできる。   In addition, after the thin battery is completed, the voltage between the current collectors 131, that is, the voltage of the bipolar electrode 13 can be measured using the remaining first conductor portion 201 and second conductor portion 202.

さらに、第１導体部２０１を封止する際に、一端を開口させておくことで完成後のガス抜き安全弁としても機能するので別途安全弁を設ける必要がない。   Furthermore, when the first conductor portion 201 is sealed, by opening one end, the first conductor portion 201 also functions as a degassing safety valve after completion, so there is no need to provide a separate safety valve.

なお、図２に示す実施形態では、チューブ２０は外装部材１５の４辺のうち正極端子プレート１１および負極端子プレート１２が導出される対向辺のそれぞれに設けたが、図６に示すように正極端子プレート１１および負極端子プレート１２が導出される辺以外の辺にチューブ２０を設けることもできる。これにより、電解液の注入やガス抜きの時間を短縮することができる。また、こうした集電体１３１へ接続しないチューブ２０は封止される機能を備えればよいので第１導体部２０１や第２導体部２０２を省略してもよい。   In the embodiment shown in FIG. 2, the tube 20 is provided on each of the opposing sides from which the positive electrode terminal plate 11 and the negative electrode terminal plate 12 are led out of the four sides of the exterior member 15, but as shown in FIG. The tube 20 can also be provided on a side other than the side from which the terminal plate 11 and the negative electrode terminal plate 12 are led out. Thereby, the time of injection | pouring of electrolyte solution and degassing can be shortened. In addition, since the tube 20 that is not connected to the current collector 131 only needs to have a sealing function, the first conductor portion 201 and the second conductor portion 202 may be omitted.

また、チューブ２０は第２シール部１４２を貫通するように設けたが、これに代えて第１シール部１４１を貫通するように設けてもよい。   Further, although the tube 20 is provided so as to penetrate the second seal portion 142, it may be provided so as to penetrate the first seal portion 141 instead.

さらに、上述した実施形態ではバイポーラ型薄型電池に適用したものを示したが、両面に正極を形成した集電体と両面に負極を形成した集電体とをセパレータを介して積層し、これを外装部材で封止するとともに、内部に電解質を封入した薄型電池にも適用することができる。この場合は、外装部材の外周のシール部に上述したチューブ２０を設ければよい。   Further, in the above-described embodiment, the present invention is applied to a bipolar thin battery. However, a current collector having a positive electrode formed on both sides and a current collector having a negative electrode formed on both surfaces are laminated via a separator, While being sealed with an exterior member, it can also be applied to a thin battery in which an electrolyte is enclosed. In this case, what is necessary is just to provide the tube 20 mentioned above in the seal part of the outer periphery of an exterior member.

また、図５Ｄに示す第１導体部２０１の封止に代えて、チューブ２０内に電池外部から電池内部への流通を阻止する逆止弁を設けることもできる。   Moreover, it can replace with sealing of the 1st conductor part 201 shown to FIG. 5D, and can also provide the check valve which prevents the distribution | circulation from the battery exterior to the battery inside in the tube 20. FIG.

上記接続部２０２Ａと封止切除部２０２Ｂが本発明の第２導体部に相当する。   The connecting portion 202A and the sealing cutout portion 202B correspond to the second conductor portion of the present invention.

１…バイポーラ薄型電池
１１…正極端子プレート
１２…負極端子プレート
１３…バイポーラ電極（発電要素）
１３１…集電体
１３２…正極
１３３…負極
１３４…セパレータ
１３５…電解液
１３６…電解質層
１３７…積層体
１４…シール部
１４１…第１シール部
１４２…第２シール部
１５…外装部材
１５１…上部外装部材
１５２…下部外装部材
２０…チューブ
２０１…第１導体部
２０２…第２導体部
２０２Ａ…接続部
２０２Ｂ…封止切除部
２０３…外筒部
Ｓ…内部空間 DESCRIPTION OF SYMBOLS 1 ... Bipolar thin battery 11 ... Positive electrode terminal plate 12 ... Negative electrode terminal plate 13 ... Bipolar electrode (power generation element)
131 ... current collector 132 ... positive electrode 133 ... negative electrode 134 ... separator 135 ... electrolyte solution 136 ... electrolyte layer 137 ... laminate 14 ... seal part 141 ... first seal part 142 ... second seal part 15 ... exterior member 151 ... upper exterior Member 152 ... Lower exterior member 20 ... Tube 201 ... First conductor portion 202 ... Second conductor portion 202A ... Connection portion 202B ... Sealed cut portion 203 ... Outer cylinder portion S ... Inner space

Claims (7)

シール部により形成された内部空間に、正極及び負極がセパレータを含む電解質層を介して積層された発電要素と、前記正極及び前記負極のそれぞれに接続された集電体とが内装された薄型電池において、
前記シール部を貫通し、一端が前記内部空間に臨み、他端が前記シール部の外部空間に臨むチューブをさらに備え、
前記チューブは、
前記内部空間に臨んで前記集電体に接続され、封止前に内部空間へ電解液を充填することができる開口面積を有するとともに押し潰して封止した後に前記チューブから前記電解液が漏洩しない厚さを有する可撓性の第１導体部と、
前記第１導体部を被覆する絶縁性外筒部と、を有することを特徴とする薄型電池。 A thin battery in which a power generation element in which a positive electrode and a negative electrode are stacked via an electrolyte layer including a separator and a current collector connected to each of the positive electrode and the negative electrode are provided in an internal space formed by the seal portion In
Further comprising a tube penetrating the seal portion, one end facing the internal space and the other end facing the external space of the seal portion;
The tube
It faces the internal space, is connected to the current collector, has an opening area that can be filled with an electrolytic solution into the internal space before sealing, and does not leak from the tube after being crushed and sealed A flexible first conductor portion having a thickness;
A thin battery comprising: an insulating outer cylinder portion covering the first conductor portion. 請求項１に記載の薄型電池において、
前記第１導体部は、前記内部空間のガス排出後にその開口が封止されることを特徴とする薄型電池。 The thin battery according to claim 1 ,
The first conductor part is a thin battery characterized in that its opening is sealed after the gas is discharged from the internal space. 請求項２に記載の薄型電池において、
前記第１導体部は、電池外部側の開口が封止され、電池内部側の開口は封止されないことを特徴とする薄型電池。 The thin battery according to claim 2 ,
The thin battery, wherein the first conductor portion has an opening on the outside of the battery sealed and an opening on the inside of the battery is not sealed. 請求項１〜３のいずれか一項に記載の薄型電池において、
複数の前記チューブを有することを特徴とする薄型電池。 In the thin battery as described in any one of Claims 1-3 ,
A thin battery comprising a plurality of the tubes. 請求項４に記載の薄型電池において、
前記薄型電池は矩形に形成され、
前記複数のチューブは、前記矩形薄型電池の少なくとも異なる辺のシール部を貫通するように配置されていることを特徴とする薄型電池。 The thin battery according to claim 4 ,
The thin battery is formed in a rectangular shape,
The thin tube is characterized in that the plurality of tubes are disposed so as to penetrate at least different side seal portions of the rectangular thin battery. 請求項１〜５のいずれか一項に記載の薄型電池において、
前記薄型電池は、集電体の一方の主面に正極が形成され他方の主面に負極が形成されたバイポーラ電極と、前記電解液が浸透するセパレータを含む電解質層と、前記バイポーラ電極と前記電解質層との間の外周を封止するシール部と、が積層されたバイポーラ電池であることを特徴とする薄型電池。 In the thin battery as described in any one of Claims 1-5 ,
The thin battery includes a bipolar electrode in which a positive electrode is formed on one main surface of a current collector and a negative electrode is formed on the other main surface, an electrolyte layer including a separator through which the electrolytic solution permeates, the bipolar electrode, A thin battery characterized in that it is a bipolar battery in which a seal part for sealing the outer periphery between the electrolyte layer and the electrolyte layer is laminated. シール部により形成された内部空間に、正極及び負極がセパレータを含む電解質層を介して積層された発電要素と、前記正極及び前記負極のそれぞれに接続された集電体とが内装された薄型電池の製造方法において、
前記内部空間に臨んで前記集電体に接続され、所定の開口面積を有するとともに押し潰して封止した後に所定の厚さを有する可撓性の第１導体部と、一端が前記第１導体部に接続され、他端が、前記シール部の外部空間に臨むとともに所定の開口面積を有する可撓性の第２導体部と、前記第１導体部および前記第２導体部を被覆する絶縁性外筒部と、を有するチューブを、その一端が前記内部空間に臨み、他端が前記シール部の外部空間に臨むように前記シール部を貫通して設ける工程と、
前記チューブの前記他端から前記内部空間へ電解液を注入する工程と、
前記第２導体部の前記他端を封止する工程と、
前記発電要素を充電する工程と、
前記第２導体部の前記他端を切除して前記チューブの前記他端を開口する工程と、
前記内部空間のガスを排出する工程と、
前記第１導体部を封止する工程と、を備えることを特徴とする薄型電池の製造方法。 A thin battery in which a power generation element in which a positive electrode and a negative electrode are stacked via an electrolyte layer including a separator and a current collector connected to each of the positive electrode and the negative electrode are provided in an internal space formed by the seal portion In the manufacturing method of
A flexible first conductor portion that faces the internal space and is connected to the current collector, has a predetermined opening area, and has a predetermined thickness after being crushed and sealed, and one end of the first conductor A flexible second conductor portion having a predetermined opening area while the other end faces the external space of the seal portion, and an insulating property that covers the first conductor portion and the second conductor portion A tube having an outer tube portion, and a step of providing the tube through the seal portion so that one end thereof faces the internal space and the other end faces the external space of the seal portion;
Injecting electrolyte from the other end of the tube into the internal space;
Sealing the other end of the second conductor portion;
Charging the power generating element;
Cutting the other end of the second conductor portion to open the other end of the tube;
Exhausting the gas in the internal space;
And a step of sealing the first conductor portion.
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