JP2002110246A - Method of producing thin battery - Google Patents

Method of producing thin battery

Info

Publication number
JP2002110246A
JP2002110246A JP2000301506A JP2000301506A JP2002110246A JP 2002110246 A JP2002110246 A JP 2002110246A JP 2000301506 A JP2000301506 A JP 2000301506A JP 2000301506 A JP2000301506 A JP 2000301506A JP 2002110246 A JP2002110246 A JP 2002110246A
Authority
JP
Japan
Prior art keywords
film material
aqueous electrolyte
exterior film
electrode group
thin battery
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
JP2000301506A
Other languages
Japanese (ja)
Inventor
Takahiro Yamamoto
高弘 山本
Yoshiaki Asami
義明 阿左美
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
A&T Battery Corp
AT Battery KK
Original Assignee
A&T Battery Corp
AT Battery KK
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by A&T Battery Corp, AT Battery KK filed Critical A&T Battery Corp
Priority to JP2000301506A priority Critical patent/JP2002110246A/en
Publication of JP2002110246A publication Critical patent/JP2002110246A/en
Pending legal-status Critical Current

Links

Classifications

    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage using batteries
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50Manufacturing or production processes characterised by the final manufactured product

Landscapes

  • Secondary Cells (AREA)

Abstract

PROBLEM TO BE SOLVED: To provide a method of producing a thin battery, using a non-aqueous electrolyte containing a non-aqueous solvent of high boiling point (>=200 deg.C) capable of uniformly impregnating non-aqueous electrolyte in a production line into a group of electrodes in an exterior film material. SOLUTION: The method of producing a thin battery comprises the process of storing the group of electrodes consisting of positive and negative electrodes wound or laminated with separators therebetween in the exterior film material consisting of plastic laminated films intervened with a gas barrier film laid in the middle and opening the exterior film material at its one end; the process of filling the non-aqueous electrolyte containing the non-aqueous solvent of a high boiling point system in the exterior film material through its opening portion under the atmospheric pressure; and the process of impregnating the non-aqueous electrolyte into the group of electrodes in the exterior film material under a reduced pressure.

Description

【発明の詳細な説明】DETAILED DESCRIPTION OF THE INVENTION

【0001】[0001]

【発明の属する技術分野】本発明は、薄型電池の製造方
法に関する。
The present invention relates to a method for manufacturing a thin battery.

【0002】[0002]

【従来の技術】近年、非水系二次電池、特にリチウムイ
オン二次電池は高電圧、高エネルギー密度を有すること
から一体型ビデオカメラ、移動通信機、ノートブック型
パソコン等のコードレスの携帯型電子機器の電源として
注目されている。とりわけ、角型二次電池の需要が伸び
ており、小型・軽量化への要求が進むに伴って電池の厚
さを薄くすることが要望されている。このような要求に
対し、小型・軽量化かつ薄型の電池の開発が盛んに行な
われている。中でも、アルミニウム箔のようなガスバリ
アフィルムを中間に挟んだプラスチックラミネートフィ
ルムを外装フィルム素材として用いる例えばポリマー電
池の研究が注目されている。
2. Description of the Related Art In recent years, non-aqueous secondary batteries, particularly lithium ion secondary batteries, have a high voltage and a high energy density. Therefore, cordless portable electronic devices such as integrated video cameras, mobile communication devices, and notebook personal computers have been developed. It is drawing attention as a power source for equipment. In particular, the demand for prismatic secondary batteries is growing, and with the demand for smaller and lighter batteries, there is a demand to reduce the thickness of the batteries. In response to such demands, small, lightweight and thin batteries have been actively developed. Above all, attention has been focused on, for example, a polymer battery using a plastic laminate film having a gas barrier film such as an aluminum foil sandwiched therebetween as an exterior film material.

【0003】ところで、従来の薄型電池は低沸点系の非
水溶媒を含む非水電解液を使用する場合、次のような方
法により製造されている。正極および負極をセパレータ
を挟んで捲回もしくは積層した電極群を中間にガスバリ
アフィルムを介在させたプラスチックラミネートフィル
ムからなる外装フィルム素材により包囲し、前記外装フ
ィルム素材を前記電極群の形状に合せて熱シールし、減
圧状態の下で非水電解液を前記外装フィルム素材に注入
した後、大気状態に戻すことにより、前記非水電解液を
前記電極群に含浸させる。
Incidentally, a conventional thin battery is manufactured by the following method when a non-aqueous electrolyte containing a non-aqueous solvent having a low boiling point is used. An electrode group in which a positive electrode and a negative electrode are wound or laminated with a separator interposed therebetween is surrounded by an exterior film material made of a plastic laminate film with a gas barrier film interposed therebetween, and the exterior film material is heated according to the shape of the electrode group. After sealing and injecting the non-aqueous electrolyte into the exterior film material under reduced pressure, the electrode group is impregnated with the non-aqueous electrolyte by returning to the atmospheric state.

【0004】[0004]

【発明が解決しようとする課題】しかしながら、前述し
た従来の方法では装置が大掛りで複雑になるばかりか、
非水電解液の電極群への含浸量がばらつくという問題が
あった。
However, in the above-mentioned conventional method, not only is the apparatus large and complicated,
There has been a problem that the impregnation amount of the non-aqueous electrolyte into the electrode group varies.

【0005】本発明は、高沸点(沸点200℃以上)の
非水溶媒を含む非水電解液を用い、簡易な製造ラインで
前記非水電解液を外装フィルム素材内の電極群に均一に
含浸することが可能な薄型電池の製造方法を提供しよう
とするものである。
The present invention uses a non-aqueous electrolyte containing a non-aqueous solvent having a high boiling point (boiling point of 200 ° C. or higher), and impregnates the non-aqueous electrolyte uniformly into a group of electrodes in an exterior film material by a simple production line. It is an object of the present invention to provide a method of manufacturing a thin battery capable of performing the above.

【0006】[0006]

【課題を解決するための手段】上記目的を達成するため
の本発明に係る薄型電池は、正極および負極をセパレー
タを挟んで捲回もしくは積層した電極群を中間にガスバ
リアフィルムを介在させたプラスチックラミネートフィ
ルムからなる外装フィルム素材に収納すると共に、その
外装フィルム素材の一端を開口する工程と、高沸点系の
非水溶媒を含む非水電解液を前記外装フィルム素材にそ
の開口部を通して大気圧下で注入する工程と、前記外装
フィルム素材を減圧雰囲気下に置いて、前記外装フィル
ム素材内の前記電極群に前記非水電解液を含浸する工程
とを具備したことを特徴とするものである。
A thin battery according to the present invention for achieving the above object is a plastic laminate in which a gas barrier film is interposed between an electrode group in which a positive electrode and a negative electrode are wound or laminated with a separator interposed therebetween. A step of opening one end of the exterior film material while storing it in the exterior film material made of a film, and applying a non-aqueous electrolyte containing a high-boiling nonaqueous solvent to the exterior film material under atmospheric pressure through the opening. A step of injecting, and a step of impregnating the non-aqueous electrolyte into the electrode group in the exterior film material by placing the exterior film material under a reduced pressure atmosphere.

【0007】本発明に係る薄型電池の製造方法におい
て、前記含浸工程における最高到達減圧度を100To
rr以下にすることが好ましい。
In the method of manufacturing a thin battery according to the present invention, the maximum attained decompression degree in the impregnation step is 100 To
It is preferable to set it to rr or less.

【0008】本発明に係る薄型電池の製造方法におい
て、前記含浸工程を減圧度をステップ状に高くすること
により行なうことが好ましい。
In the method for manufacturing a thin battery according to the present invention, it is preferable that the impregnation step is performed by increasing the degree of pressure reduction stepwise.

【0009】本発明に係る薄型電池の製造方法におい
て、前記含浸工程後に前記外装フィルム素材の開口部を
熱シールする際、減圧下で行なって前記電極群および非
水電解液を外装フィルム内に密閉すること許容する。
In the method of manufacturing a thin battery according to the present invention, when the opening of the exterior film material is heat-sealed after the impregnation step, the electrode group and the non-aqueous electrolyte are hermetically sealed in the exterior film. Tolerate.

【0010】[0010]

【発明の実施の形態】以下、本発明に係る薄型電池の製
造方法図1〜図6を参照して詳細に説明する。
DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS Hereinafter, a method for manufacturing a thin battery according to the present invention will be described in detail with reference to FIGS.

【0011】(第1工程)まず、正極、セパレータ、負
極およびセパレータを渦巻き状に捲回してほぼ円筒状に
した後、例えば室温で加圧成形することにより図1およ
び図2に示すように正極1、セパレータ2、負極3およ
びセパレータ2を渦巻き状に捲回され、扁平で矩形状を
なす電極群4を作製する。なお、前記捲回に先立って正
負極1,3に外部端子5,6をそれぞれ例えば超音波溶
接により接続する。つづいて、二つ折りのカップ型外装
フィルム素材を用意し、この外装フィルム素材7のカッ
プ8内に前記扁平状の電極群4をその外部端子5,6の
反対側の面が前記外装フィルム素材の折り曲げ部側に位
置するように収納する。前記外装フィルム素材7は、内
面側に位置するシーラントフィルム、例えばアルミニウ
ム箔のようなガスバリアフィルムおよび剛性を有する有
機樹脂フィルムをこの順序で積層した構造を有する。ひ
きつづき、前記電極群4の長辺に対応する前記外装フィ
ルム素材7の左端部および前記外部端子5,6の延出側
に対応する前記素材7の端部を熱シールしてシール部9
a,9bを形成することにより図3に示すように前記電
極群4の長辺と平行する端部が未シール部(開口部)1
0とした袋状外装フィルム素材11とする。
(First Step) First, the positive electrode, the separator, the negative electrode, and the separator are spirally wound into a substantially cylindrical shape, and then subjected to pressure molding at room temperature, for example, as shown in FIG. 1 and FIG. 1, a separator 2, a negative electrode 3, and a separator 2 are spirally wound to produce a flat and rectangular electrode group 4. Prior to the winding, external terminals 5 and 6 are connected to the positive and negative electrodes 1 and 3, respectively, for example, by ultrasonic welding. Subsequently, a two-fold cup-shaped exterior film material is prepared, and the flat electrode group 4 is placed in the cup 8 of the exterior film material 7 so that the surface opposite to the external terminals 5 and 6 is formed of the exterior film material. It is stored so as to be located on the bent part side. The exterior film material 7 has a structure in which a sealant film located on the inner surface side, for example, a gas barrier film such as an aluminum foil and a rigid organic resin film are laminated in this order. Subsequently, the left end of the exterior film material 7 corresponding to the long side of the electrode group 4 and the end of the material 7 corresponding to the extension side of the external terminals 5 and 6 are heat-sealed to form a sealing portion 9.
By forming the a and 9b, the end parallel to the long side of the electrode group 4 becomes an unsealed portion (opening) 1 as shown in FIG.
The bag-shaped exterior film material 11 was set to 0.

【0012】前記正極、セパレータ、負極およびセパレ
ータを渦巻き状に捲回するための捲回機および巻芯は、
特に限定されないが、巻芯には円柱状、楕円柱状、平板
状、菱形状等のものを用いることができる。
A winding machine and a winding core for spirally winding the positive electrode, the separator, the negative electrode and the separator include:
Although not particularly limited, a core having a columnar shape, an elliptical columnar shape, a flat plate shape, a diamond shape, or the like can be used.

【0013】前記電極群を扁平状に成形するためのプレ
ス機は、特に限定されないが、電極群に均一な加圧力を
与えることが可能な一軸成形法が好ましい。
The press for forming the electrode group into a flat shape is not particularly limited, but a uniaxial forming method capable of applying a uniform pressing force to the electrode group is preferable.

【0014】(第2工程)図3に示すように袋状外装フ
ィルム素材11の開口部10を拡口し、この開口部10
に非水電解液を大気圧下で例えば注入ノズル12を通し
て所定量注入する。つづいて、図4に示すように図示し
ないバルブが介装された排気管13および図示しないバ
ルブが介装された大気導入管14が側壁に接続された角
型真空チャンバ15を用意し、この真空チャンバ15内
に大気圧下で非水電解液が注入された複数の袋状外装フ
ィルム素材11をそれぞれ設置し、前記排気管13に接
続された真空ポンプ(図示せず)を作動して前記真空チ
ャンバ15内を所定の減圧度にすることにより前記複数
の袋状外装フィルム11内の非水電解液を電極群4に含
浸させる。
(Second Step) As shown in FIG. 3, the opening 10 of the bag-shaped exterior film material 11 is widened, and this opening 10
A predetermined amount of a non-aqueous electrolyte is injected under atmospheric pressure through, for example, an injection nozzle 12. Subsequently, as shown in FIG. 4, a rectangular vacuum chamber 15 in which an exhaust pipe 13 in which a valve (not shown) is interposed and an air introducing pipe 14 in which a valve (not shown) is interposed is connected to a side wall is prepared. A plurality of bag-shaped exterior film materials 11 into which a non-aqueous electrolyte is injected under atmospheric pressure are installed in a chamber 15, and a vacuum pump (not shown) connected to the exhaust pipe 13 is operated to operate the vacuum. The electrode group 4 is impregnated with the non-aqueous electrolyte in the plurality of bag-shaped exterior films 11 by reducing the pressure in the chamber 15 to a predetermined degree.

【0015】前記非水電解液の含浸工程において、前記
排気管13に介装した図示しないバルブおよび前記大気
導入管14に介装した図示しないバルブの開度をそれぞ
れコントロールして前記真空チャンバ15内をステップ
状に減圧にすることが好ましい。また、前記真空チャン
バ15内の最大到達減圧度は100Torr以下、より
好ましくは50Torr以下にすることが望ましい。
In the impregnation step of the non-aqueous electrolyte, the degree of opening of a valve (not shown) provided in the exhaust pipe 13 and a valve (not shown) provided in the atmosphere introducing pipe 14 are controlled to control the degree of opening of the vacuum chamber 15. Is preferably reduced stepwise. Further, it is preferable that the maximum attained decompression degree in the vacuum chamber 15 is 100 Torr or less, more preferably 50 Torr or less.

【0016】(第3工程)前記含浸工程後に前記開口部
10側の電極群4の長辺近傍に位置する前記袋状外装フ
ィルム素材11部分を前記開口部10に平行して熱シー
ルし、さらに不要なフィルム素材11部分を切断するこ
とにより、図5、図6に示すようにシーラントフィルム
16、ガスバリアフィルム17および剛性を有する有機
樹脂フィルム18がこの順序で積層され、3つの辺にシ
ール部9a,9b,9cを有する外装フィルム19内に
非水電解液が含浸された電極群4を密封した構造の薄型
二次電池を製造する。
(Third Step) After the impregnating step, the bag-like exterior film material 11 located near the long side of the electrode group 4 on the opening 10 side is heat-sealed in parallel with the opening 10, By cutting off the unnecessary film material 11, a sealant film 16, a gas barrier film 17 and a rigid organic resin film 18 are laminated in this order as shown in FIGS. , 9b, and 9c, a thin secondary battery having a structure in which the electrode group 4 in which the nonaqueous electrolyte is impregnated in the exterior film 19 is sealed.

【0017】前記熱シール工程は、減圧状態で行なうこ
とが好ましい。
Preferably, the heat sealing step is performed under reduced pressure.

【0018】次に、前記正極1、セパレータ2、負極
3、非水電解液および外装フィルム5を説明する。
Next, the positive electrode 1, the separator 2, the negative electrode 3, the non-aqueous electrolyte and the outer film 5 will be described.

【0019】前記正極1は、集電体の片面もしくは両面
に活物質を含む正極活物質層を形成した構造を有する。
The positive electrode 1 has a structure in which a positive electrode active material layer containing an active material is formed on one or both surfaces of a current collector.

【0020】前記集電体としては、例えばアルミニウ
ム、ニッケルまたはステンレスの板、アルミニウム、ニ
ッケルまたはステンレスのメッシュ等を挙げることがで
きる。
Examples of the current collector include a plate of aluminum, nickel or stainless steel, and a mesh of aluminum, nickel or stainless steel.

【0021】前記正極活物質としては、種々の酸化物、
例えば二酸化マンガン、リチウムマンガン複合酸化物、
リチウム含有ニッケル酸化物、リチウム含有コバルト化
合物、リチウム含有ニッケルコバルト酸化物、リチウム
含有鉄酸化物、リチウムを含むバナジウム酸化物や、二
硫化チタン、二硫化モリブデンなどのカルコゲン化合物
などを挙げることができる。中でも、リチウムコバルト
酸化物(LiCoO2)、リチウムニッケル酸化物(L
iNiO2 )、リチウムマンガン酸化物(LiMn2
4 またはLiMnO2 )を用いると、高電圧が得られる
ために好ましい。
As the positive electrode active material, various oxides,
For example, manganese dioxide, lithium manganese composite oxide,
Examples include lithium-containing nickel oxide, lithium-containing cobalt compound, lithium-containing nickel-cobalt oxide, lithium-containing iron oxide, lithium-containing vanadium oxide, and chalcogen compounds such as titanium disulfide and molybdenum disulfide. Among them, lithium cobalt oxide (LiCoO 2 ) and lithium nickel oxide (L
iNiO 2 ), lithium manganese oxide (LiMn 2 O)
4 or LiMnO 2 ) is preferable because a high voltage can be obtained.

【0022】前記正極活物質層は、結着剤および導電剤
を含有することが好ましい。
The positive electrode active material layer preferably contains a binder and a conductive agent.

【0023】前記結着剤としては、例えばポリテトラフ
ルオロエチレン(PTFE)、ポリフッ化ビニリデン
(PVDF)、エチレン−プロピレン−ジエン共重合体
(EPDM)、スチレン−ブタジエンゴム(SBR)等
を用いることができる。
Examples of the binder include polytetrafluoroethylene (PTFE), polyvinylidene fluoride (PVDF), ethylene-propylene-diene copolymer (EPDM), and styrene-butadiene rubber (SBR). it can.

【0024】前記導電剤としては、例えばアセチレンブ
ラック、カーボンブラック、黒鉛等を挙げることができ
る。
Examples of the conductive agent include acetylene black, carbon black, graphite and the like.

【0025】前記正極から取り出される外部端子の主た
る材質は、アルミニウムであることが好ましい。また、
前記外装フィルムとのシール性を向上するために前記外
部端子に化学的または物理的な表面処理を行なうことが
より好ましい。
The main material of the external terminal taken out from the positive electrode is preferably aluminum. Also,
It is more preferable to perform a chemical or physical surface treatment on the external terminals in order to improve the sealing property with the exterior film.

【0026】前記セパレータ2としては、例えばポリエ
チレン、ポリプロピレン、エチレン−プロピレン共重合
体、エチレン−ブテン共重合体からなる微多孔性膜また
はこれら材料の繊維を有する織布、不織布により作られ
る。
The separator 2 is made of, for example, a microporous film made of polyethylene, polypropylene, ethylene-propylene copolymer, ethylene-butene copolymer, or a woven or nonwoven fabric having fibers of these materials.

【0027】前記負極3は、集電体の少なくとも片面に
活物質を含む負極活物質層を形成した構造を有する。
The negative electrode 3 has a structure in which a negative electrode active material layer containing an active material is formed on at least one surface of a current collector.

【0028】前記集電体としては、例えば銅板、銅メッ
シュ等を挙げることができる。
Examples of the current collector include a copper plate and a copper mesh.

【0029】前記負極活物質は、特に限定されないが、
金属リチウム、リチウム合金、または充放電時にリチウ
ムイオンを可逆的に吸蔵・放出、もしくはインターカレ
ート・ディインターカレートするコークス、炭素繊維、
黒鉛、メソフェーズピッチ系炭素、熱分解気相炭素質
物、樹脂焼成体等の炭素質材料等を挙げることができ
る。
The negative electrode active material is not particularly limited.
Lithium metal, lithium alloy, or coke or carbon fiber that reversibly inserts or releases lithium ions during charge / discharge, or intercalates / deintercalates,
Examples include graphite, mesophase pitch-based carbon, pyrolytic gas-phase carbonaceous materials, and carbonaceous materials such as resin fired bodies.

【0030】前記負極活物質層は、例えば結着剤を含有
することが好ましい。
The negative electrode active material layer preferably contains, for example, a binder.

【0031】前記結着剤としては、例えばポリテトラフ
ルオロエチレン、ポリビニリデンフルオロライド、エチ
レン−プロピレン−ジエン共重合体、スチレン−ブタジ
エンゴム、カルボキシメチルセルロース等の結着剤を含
有することが好ましい。
The binder preferably contains, for example, a binder such as polytetrafluoroethylene, polyvinylidene fluoride, ethylene-propylene-diene copolymer, styrene-butadiene rubber, and carboxymethyl cellulose.

【0032】前記負極から取り出される外部端子の主た
る材質は、ニッケルであることが好ましい。また、前記
外装フィルムとのシール性を向上するために前記外部端
子に化学的または物理的な表面処理を行なうことがより
好ましい。
The main material of the external terminal taken out from the negative electrode is preferably nickel. Further, it is more preferable to perform a chemical or physical surface treatment on the external terminals in order to improve the sealing property with the exterior film.

【0033】前記外装フィルム素材7のシーラントフィ
ルムとしては、例えばポリエチレン(PE)フィルム、
ポリプロピレン(PP)フィルム、ポリプロピレン−ポ
リエチレン共重合体フィルム、アイオノマーフィルム、
エチレンビニルアセテート(EVA)フィルム等を用い
ることができる。前記剛性を有する有機樹脂フィルムと
しては、例えばポリエチレンテレフタレート(PET)
フィルム、ナイロンフィルム等を用いることができる。
As the sealant film of the exterior film material 7, for example, a polyethylene (PE) film,
Polypropylene (PP) film, polypropylene-polyethylene copolymer film, ionomer film,
An ethylene vinyl acetate (EVA) film or the like can be used. As the rigid organic resin film, for example, polyethylene terephthalate (PET)
Films, nylon films and the like can be used.

【0034】前記シーラントフィルム、アルミニウム箔
および有機樹脂フィルムの厚さは、特に限定されない
が、シーラントフィルムは20〜100μm、アルミニ
ウム箔は20〜80μm、有機樹脂フィルム10〜10
0μmにすることが好ましい。
The thickness of the sealant film, the aluminum foil and the organic resin film is not particularly limited, but is 20 to 100 μm for the sealant film, 20 to 80 μm for the aluminum foil, 10 to 10 μm for the organic resin film.
Preferably, the thickness is 0 μm.

【0035】前記非水電解液は、電解質を非水溶媒で溶
解した組成を有する。
The non-aqueous electrolyte has a composition in which an electrolyte is dissolved in a non-aqueous solvent.

【0036】電解質としては、例えば過塩素酸リチウム
(LiClO4)、四フッ化硼酸リチウム(LiB
4)、六フッ化燐酸リチウム(LiPF6)、六フッ化
砒素酸リチウム(LiAsF6)、トリフルオロメタン
スルホン酸リチウム(LiCF3SO3)、LiN(CF
3SO22等を用いることができる。
As the electrolyte, for example, lithium perchlorate (LiClO 4 ), lithium tetrafluoroborate (LiB
F 4 ), lithium hexafluorophosphate (LiPF 6 ), lithium hexafluoroarsenate (LiAsF 6 ), lithium trifluoromethanesulfonate (LiCF 3 SO 3 ), LiN (CF
3 SO 2 ) 2 or the like can be used.

【0037】非水溶媒としては、沸点が200℃以上の
高沸点系であればいずれのものも使用でき、例えばエチ
レンカーボネート、プロピレンカーボネート、ブチレン
カーボネート、γ−ブチロラクトン、スルホラン、3−
メチルスルホラン、テトラエチレングリコールジメチル
エーテル、トリエチレングリコールジメチルエーテル、
メチルトリグライム、ブチルジグライム等を用いること
ができる。これらの非水溶媒は、1種または2種以上の
混合物の形態で用いることができる。
As the non-aqueous solvent, any high-boiling system having a boiling point of 200 ° C. or more can be used. For example, ethylene carbonate, propylene carbonate, butylene carbonate, γ-butyrolactone, sulfolane,
Methylsulfolane, tetraethylene glycol dimethyl ether, triethylene glycol dimethyl ether,
Methyl triglyme, butyl diglyme and the like can be used. These non-aqueous solvents can be used in the form of one kind or a mixture of two or more kinds.

【0038】前記非水電解液は、通常、溶液の形態で用
いられるが、固体状(例えばゾル状、ゲル状等)、また
は固体状と溶液状の混合形態でもよい。
The non-aqueous electrolyte is usually used in the form of a solution, but may be in the form of a solid (for example, a sol, a gel or the like) or a mixture of a solid and a solution.

【0039】前記非水溶媒中の前記電解質の濃度は、
0.5モル/L以上にすることが好ましい。
The concentration of the electrolyte in the non-aqueous solvent is as follows:
It is preferable to set it to 0.5 mol / L or more.

【0040】前記電極群は、前述した扁平状のものに限
らず、正極、セパレータおよび負極を積層した構造のも
のでもよい。
The electrode group is not limited to the flat one described above, but may have a structure in which a positive electrode, a separator and a negative electrode are laminated.

【0041】本発明に係わる薄型電池の製造において、
外装フィルム素材は図1に示すカップ型に限らず、折り
曲げシール部を有するピロー構造の外装フィルム素材、
パウチ型の外装フィルム素材を用いてもよい。
In the manufacture of the thin battery according to the present invention,
The exterior film material is not limited to the cup type shown in FIG. 1, but an exterior film material having a pillow structure having a bent seal portion,
A pouch-type exterior film material may be used.

【0042】以上説明したように、本発明の薄型電池の
製造方法は正極および負極をセパレータを挟んで捲回も
しくは積層した電極群を中間にガスバリアフィルムを介
在させたプラスチックラミネートフィルムからなる外装
フィルム素材に収納すると共に、その外装フィルム素材
の一端を開口する工程と、高沸点系の非水溶媒を含む非
水電解液を前記外装フィルム素材にその開口部を通して
大気圧下で注入する工程と、前記外装フィルム素材を減
圧雰囲気下に置いて、前記外装フィルム素材内の前記電
極群に前記非水電解液を含浸する工程とを具備する。
As described above, the method of manufacturing a thin battery according to the present invention provides an exterior film material composed of a plastic laminate film having a gas barrier film interposed between an electrode group in which a positive electrode and a negative electrode are wound or laminated with a separator interposed therebetween. Along with storing in the exterior film material, a step of opening one end of the exterior film material, and a step of injecting a non-aqueous electrolyte containing a high-boiling nonaqueous solvent into the exterior film material under atmospheric pressure through the opening portion, Placing the exterior film material under a reduced-pressure atmosphere and impregnating the electrode group in the exterior film material with the non-aqueous electrolyte.

【0043】このような方法によれば、高沸点系の非水
溶媒を含む非水電解液を用いることによって、大気圧下
で前記外装フィルム素材に注入することができるため、
製造ラインが簡易になり、電極群に非水電解液を液量の
ばらつきを生じることなく円滑に含浸することができ
る。
According to such a method, by using a non-aqueous electrolyte containing a non-aqueous solvent having a high boiling point, the non-aqueous electrolyte can be injected into the exterior film material under atmospheric pressure.
The production line is simplified, and the electrode group can be smoothly impregnated with the non-aqueous electrolyte without causing a variation in the amount of the solution.

【0044】また、前記含浸工程後に前記外装フィルム
素材の開口部を熱シールする際、減圧下で行なって前記
電極群および非水電解液を外装フィルム内に密閉するこ
とによって、厚さがより薄い薄型電池を製造できる。
When the opening of the exterior film material is heat-sealed after the impregnation step, the thickness is reduced by sealing the group of electrodes and the non-aqueous electrolyte in the exterior film by performing the process under reduced pressure. Thin batteries can be manufactured.

【0045】さらに、前記含浸工程において雰囲気中の
減圧度を制御して減圧度をステップ状に高くすることに
よって前記外装フィルム素材に注入した非水電解液の吹
き出しを抑制しつつ、非水電解液を電極群に含浸するこ
とができる。その上、前記含浸工程後に前記外装フィル
ム素材の開口部を減圧下で熱シールする際、非水電解液
の外装フィルム素材からの突沸を抑制することができ
る。
Further, in the impregnation step, the degree of pressure reduction in the atmosphere is controlled so as to increase the degree of pressure reduction in a step-like manner, thereby preventing the non-aqueous electrolyte solution injected into the exterior film material from being blown out. Can be impregnated into the electrode group. In addition, when the opening of the exterior film material is heat-sealed under reduced pressure after the impregnation step, bumping of the non-aqueous electrolyte from the exterior film material can be suppressed.

【0046】[0046]

【実施例】以下、本発明の好ましい実施例を前述した図
面を参照して説明する。
Preferred embodiments of the present invention will be described below with reference to the accompanying drawings.

【0047】(実施例1) <正極の作製>まず、活物質としてのLiCoO2粉末
89重量部に導電フィラーとしてのグラファイト粉末8
重量部および結着剤としてポリフッ化ビニリデン樹脂3
重量部をN−メチルピロリドン25重量部に混合してペ
ーストを調製した。このペーストを外部端子が取付けら
れたアルミニウム箔の両面に塗布し、乾燥し、さらにプ
レス加工、スリット加工を施してリール状の正極を作製
した。
Example 1 <Preparation of Positive Electrode> First, graphite powder 8 as a conductive filler was added to 89 parts by weight of LiCoO 2 powder as an active material.
Parts by weight and polyvinylidene fluoride resin 3 as a binder
Parts by weight was mixed with 25 parts by weight of N-methylpyrrolidone to prepare a paste. This paste was applied to both sides of an aluminum foil to which external terminals were attached, dried, and then subjected to press working and slit processing to produce a reel-shaped positive electrode.

【0048】<負極の作製>まず、鱗片状グラファイト
カーボン100重量部をカルボキシメチルセルロースお
よびスチレン−ブタジエンの架橋ゴムラテックス粒子2
重量部を含む水溶液に混合してペーストを調製した。こ
のペーストを外部端子が取付けられた銅箔の両面に塗布
し、乾燥し、さらにプレス加工、スリット加工を施して
リール状の負極を作製した。
<Preparation of Negative Electrode> First, 100 parts by weight of flaky graphite carbon was mixed with carboxymethyl cellulose and styrene-butadiene crosslinked rubber latex particles 2
It was mixed with an aqueous solution containing parts by weight to prepare a paste. This paste was applied to both sides of the copper foil to which the external terminals were attached, dried, and then subjected to press working and slit processing to produce a reel-shaped negative electrode.

【0049】<非水電解液>エチレンカーボネートとγ
−ブチロラクトンを1:1の体積比で混合した高沸点系
混合溶媒(沸点205℃)に四フッ化硼酸リチウム(L
iBF4)を1モル/L溶解して非水電解液を調製し
た。
<Non-aqueous electrolyte> Ethylene carbonate and γ
Lithium tetrafluoroborate (L) was added to a high-boiling mixed solvent (boiling point 205 ° C.) in which butyrolactone was mixed at a volume ratio of 1: 1.
iBF 4 ) was dissolved at 1 mol / L to prepare a non-aqueous electrolyte.

【0050】次いで、前記正負極の間および正極側にポ
リエチレン製微多孔膜を配置し、正負極にアルミニウム
製外部端子を、負極にニッケル製外部端子をそれぞれ接
続した後、捲回機により前記正極のアルミニウム箔が最
外周に位置するように渦巻き状に捲回して円筒状物を作
成した。つづいて、この円筒状物を80℃、15kgf
/cm2の圧力で加熱加圧成形することにより扁平状を
なす電極群を作製した。
Next, a polyethylene microporous membrane is disposed between the positive and negative electrodes and on the positive electrode side, and an aluminum external terminal is connected to the positive and negative electrodes, and a nickel external terminal is connected to the negative electrode. The aluminum foil was spirally wound so that the aluminum foil was positioned at the outermost periphery to form a cylindrical object. Subsequently, this cylindrical object is heated at 80 ° C. and 15 kgf
An electrode group having a flat shape was produced by heating and pressing at a pressure of / cm 2 .

【0051】次いで、二つ折りされたカップ型外装フィ
ルム素材(シーラントフィルム、アルミニウム箔および
ナイロンフィルムのラミネートフィルム)を用意し、こ
の外装フィルム素材のカップ内に前記扁平状電極群をそ
の外部端子の反対側の面が前記外装フィルム素材の折り
曲げ部側に位置するように収納した。つづいて、前記電
極群の長辺に対応する前記外装フィルム素材の左端部お
よび前記各外部端子の延出側に対応する前記素材の端部
を熱シールしてシール部を形成することにより前記電極
群の長辺と平行する端部が未シール部(開口部)とした
袋状外装フィルム素材を作製した。
Next, a cup-shaped exterior film material (a laminate film of a sealant film, an aluminum foil and a nylon film) which is folded in two is prepared, and the flat electrode group is placed in a cup of the exterior film material opposite to its external terminals. The outer film material was housed so that its side surface was located on the bent portion side of the exterior film material. Subsequently, the left end of the exterior film material corresponding to the long side of the electrode group and the end of the material corresponding to the extension side of each of the external terminals are heat-sealed to form a seal portion, thereby forming the electrode. A bag-shaped exterior film material in which an end parallel to the long side of the group was an unsealed portion (opening) was produced.

【0052】次いで、前記袋状外装フィルム素材の開口
部を拡口し、この開口部に前記組成の非水電解液3.2
0gを大気圧下で注入ノズルを通して注入した。つづい
て、角型真空チャンバ内に複数の前記袋状外装フィルム
素材をそれぞれ設置し、前記チャンバの排気管に接続さ
れた真空ポンプを作動すると共に、その排気管に介装さ
れたバルブの開閉および前記チャンバの大気導入管に介
装されたバルブの開閉を行なって、減圧・大気開放を繰
り返して前記チャンバ内の減圧度をステップ状に上げて
最大到達減圧度50Torrにすることにより前記袋状
外装フィルム素材において非水電解液を電極群に含浸さ
せた。ひきつづき、減圧状態で前記開口部側の電極群の
長辺近傍に位置する前記袋状外装フィルム素材部分を前
記開口部に平行して熱シールし、さらに不要なフィルム
素材部分を切断することにより、図5、図6に示すよう
に外装フィルム19内に非水電解液が含浸された電極群
4を密封した構造を有する20個の薄型二次電池を製造
した。
Next, the opening of the bag-shaped exterior film material was widened, and the nonaqueous electrolytic solution 3.2 having the above composition was formed in the opening.
0 g were injected at atmospheric pressure through the injection nozzle. Subsequently, a plurality of the bag-shaped exterior film materials are respectively installed in a rectangular vacuum chamber, and a vacuum pump connected to an exhaust pipe of the chamber is operated, and opening and closing of a valve interposed in the exhaust pipe and The bag-shaped exterior is opened and closed by repeatedly opening and closing a valve interposed in an air introduction pipe of the chamber, and increasing the decompression degree in the chamber in steps by reducing and opening the air to the maximum decompression degree of 50 Torr. The electrode group was impregnated with a non-aqueous electrolyte in a film material. Subsequently, the bag-shaped exterior film material portion located in the vicinity of the long side of the electrode group on the opening side under reduced pressure is heat-sealed in parallel with the opening, and further unnecessary film material portions are cut, As shown in FIGS. 5 and 6, 20 thin secondary batteries having a structure in which the electrode group 4 in which the non-aqueous electrolyte was impregnated in the outer film 19 were sealed were manufactured.

【0053】(比較例1)非水電解液としてエチレンカ
ーボネートおよびメチルエチルカーボネートを1:1の
体積比混合した混合溶媒(沸点110℃)に六フッ化燐
酸リチウム(LiPF6)を1モル/L溶解して調製し
たものを用いた以外、実施例1と同様な方法により20
個の薄型非水電解液二次電池を製造した。
Comparative Example 1 As a non-aqueous electrolyte, 1 mol / L of lithium hexafluorophosphate (LiPF 6 ) was mixed with a mixed solvent (boiling point: 110 ° C.) in which ethylene carbonate and methyl ethyl carbonate were mixed at a volume ratio of 1: 1. Except for using a solution prepared by dissolving, 20
Two thin non-aqueous electrolyte secondary batteries were manufactured.

【0054】得られた実施例1および比較例1の20個
の薄型非水電解液二次電池について、非水電解液の注
入、含浸前と非水電解液含浸後の二次電池の重量を測定
することにより含浸後の非水電解液の重量を求めた。そ
の結果を下記表1に示す。
For the 20 thin non-aqueous electrolyte secondary batteries of Example 1 and Comparative Example 1, the weight of the secondary batteries before injection and impregnation of the non-aqueous electrolyte and after impregnation with the non-aqueous electrolyte were measured. The weight of the non-aqueous electrolyte after impregnation was determined by measurement. The results are shown in Table 1 below.

【0055】[0055]

【表1】 [Table 1]

【0056】前記表1から明らかなように実施例1の薄
型非水電解液二次電池は、電極群に含浸される非水電解
液量のばらつきが比較例1の低沸点の非水電解液を用い
る薄型非水電解液二次電池に比べて極めて小さく、安定
した非水電解液の注入・含浸がなされ、高沸点系の非水
電解液の含浸に有効であることがわかる。
As is clear from Table 1, the thin non-aqueous electrolyte secondary battery of Example 1 has a low boiling point non-aqueous electrolyte of Comparative Example 1 in which the amount of non-aqueous electrolyte impregnated in the electrode group varies. It can be seen that injection and impregnation of a non-aqueous electrolyte are extremely small and stable compared with a thin non-aqueous electrolyte secondary battery using, and it is effective for impregnation with a high-boiling non-aqueous electrolyte.

【0057】[0057]

【発明の効果】以上詳述したように、本発明によれば高
沸点(沸点200℃以上)の非水溶媒を含む非水電解液
を用い、簡易な製造ラインで前記非水電解液を外装フィ
ルム素材内の電極群に均一に含浸することが可能で、一
体型ビデオカメラ、移動通信機、ノートブック型パソコ
ン等のコードレスの携帯型電子機器の電源等に有効な薄
型電池の製造方法を提供できる。
As described above in detail, according to the present invention, a non-aqueous electrolyte containing a non-aqueous solvent having a high boiling point (boiling point of 200 ° C. or more) is used, and the non-aqueous electrolyte is packaged on a simple production line. Provides a method of manufacturing a thin battery that can uniformly impregnate the electrodes in a film material and is effective as a power source for cordless portable electronic devices such as integrated video cameras, mobile communication devices, and notebook computers. it can.

【図面の簡単な説明】[Brief description of the drawings]

【図1】本発明に係わる薄型非水電解液二次電池の製造
工程を示す斜視図。
FIG. 1 is a perspective view showing a manufacturing process of a thin non-aqueous electrolyte secondary battery according to the present invention.

【図2】図1のII−II線に沿う断面図。FIG. 2 is a sectional view taken along the line II-II in FIG.

【図3】本発明に係わる薄型非水電解液二次電池の製造
工程を示す斜視図。
FIG. 3 is a perspective view showing a manufacturing process of the thin non-aqueous electrolyte secondary battery according to the present invention.

【図4】本発明に係わる薄型非水電解液二次電池の製造
に用いられる角型真空チャンバを示す斜視図。
FIG. 4 is a perspective view showing a rectangular vacuum chamber used for manufacturing a thin non-aqueous electrolyte secondary battery according to the present invention.

【図5】本発明に係る方法により製造された薄型非水電
解液二次電池を示す斜視図。
FIG. 5 is a perspective view showing a thin non-aqueous electrolyte secondary battery manufactured by the method according to the present invention.

【図6】図5のVI−VI線に沿う断面図。FIG. 6 is a sectional view taken along the line VI-VI in FIG. 5;

【符号の説明】[Explanation of symbols]

1…正極、 2…セパレータ、 3…負極、 4…電極群、 5,6…外部端子、 7…外装フィルム素材、 9a,9b,9c…シール部、 11…袋状外装フィルム素材、 15…角型真空チャンバ、 16…シーラントフィルム、 17…ガスバリアフィルム、 18…剛性を有する有機樹脂フィルム 19…外装フィルム。 DESCRIPTION OF SYMBOLS 1 ... Positive electrode, 2 ... Separator, 3 ... Negative electrode, 4 ... Electrode group, 5, 6 ... External terminal, 7 ... Exterior film material, 9a, 9b, 9c ... Seal part, 11 ... Bag-shaped exterior film material, 15 ... Square Mold vacuum chamber, 16: sealant film, 17: gas barrier film, 18: organic resin film having rigidity 19: exterior film

Claims (4)

【特許請求の範囲】[Claims] 【請求項1】 正極および負極をセパレータを挟んで捲
回もしくは積層した電極群を中間にガスバリアフィルム
を介在させたプラスチックラミネートフィルムからなる
外装フィルム素材に収納すると共に、その外装フィルム
素材の一端を開口する工程と、 高沸点系の非水溶媒を含む非水電解液を前記外装フィル
ム素材にその開口部を通して大気圧下で注入する工程
と、 前記外装フィルム素材を減圧雰囲気下に置いて、前記外
装フィルム素材内の前記電極群に前記非水電解液を含浸
する工程とを具備したことを特徴とする薄型電池の製造
方法。
An electrode group in which a positive electrode and a negative electrode are wound or laminated with a separator interposed therebetween is housed in an exterior film material made of a plastic laminate film with a gas barrier film interposed therebetween, and one end of the exterior film material is opened. And a step of injecting a non-aqueous electrolyte containing a non-aqueous solvent having a high boiling point into the exterior film material under atmospheric pressure through the opening thereof. Impregnating the non-aqueous electrolyte into the electrode group in a film material.
【請求項2】 前記含浸工程における最高到達減圧度
は、100Torr以下であることを特徴とする請求項
1記載の薄型電池の製造方法。
2. The method for manufacturing a thin battery according to claim 1, wherein a maximum ultimate pressure reduction degree in the impregnation step is 100 Torr or less.
【請求項3】 前記含浸工程は、減圧度をステップ状に
高くすることによりなされることを特徴とする請求項1
または2記載の薄型電池の製造方法。
3. The method according to claim 1, wherein the impregnating step is performed by increasing the degree of decompression stepwise.
Or a method for manufacturing a thin battery according to 2.
【請求項4】 前記含浸工程後に前記外装フィルム素材
の開口部を熱シールする際、減圧下で行なって前記電極
群および非水電解液を外装フィルム内に密閉することを
特徴とする請求項1ないし3いずれか記載の薄型電池の
製造方法。
4. The method according to claim 1, wherein the heat sealing of the opening of the exterior film material after the impregnation step is performed under reduced pressure to seal the electrode group and the non-aqueous electrolyte in the exterior film. 4. The method for producing a thin battery according to any one of items 3 to 3.
JP2000301506A 2000-09-29 2000-09-29 Method of producing thin battery Pending JP2002110246A (en)

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Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2008071496A (en) * 2006-09-12 2008-03-27 Enax Inc Sheet-shaped secondary battery and its manufacturing method
KR101043847B1 (en) 2003-02-28 2011-06-22 에프디케이 가부시키가이샤 Heat-Resistant Lithium Battery
KR20120013901A (en) * 2010-08-06 2012-02-15 소니 주식회사 Battery and method for producing the same

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Publication number Priority date Publication date Assignee Title
JPH10270072A (en) * 1997-03-21 1998-10-09 Japan Storage Battery Co Ltd Manufacture of nonaqueous electrolyte secondary battery
JPH10302827A (en) * 1997-04-24 1998-11-13 Nec Corp Manufacture of electrode group of angular battery
JPH11307133A (en) * 1998-02-19 1999-11-05 Matsushita Electric Ind Co Ltd Manufacture of organic electrolyte battery
WO2000041263A1 (en) * 1998-12-28 2000-07-13 Mitsubishi Denki Kabushiki Kaisha Thin battery and method of manufacturing
JP2000200587A (en) * 1999-01-04 2000-07-18 Mitsubishi Electric Corp Battery and its manufacture

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH10270072A (en) * 1997-03-21 1998-10-09 Japan Storage Battery Co Ltd Manufacture of nonaqueous electrolyte secondary battery
JPH10302827A (en) * 1997-04-24 1998-11-13 Nec Corp Manufacture of electrode group of angular battery
JPH11307133A (en) * 1998-02-19 1999-11-05 Matsushita Electric Ind Co Ltd Manufacture of organic electrolyte battery
WO2000041263A1 (en) * 1998-12-28 2000-07-13 Mitsubishi Denki Kabushiki Kaisha Thin battery and method of manufacturing
JP2000200587A (en) * 1999-01-04 2000-07-18 Mitsubishi Electric Corp Battery and its manufacture

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
KR101043847B1 (en) 2003-02-28 2011-06-22 에프디케이 가부시키가이샤 Heat-Resistant Lithium Battery
JP2008071496A (en) * 2006-09-12 2008-03-27 Enax Inc Sheet-shaped secondary battery and its manufacturing method
KR20120013901A (en) * 2010-08-06 2012-02-15 소니 주식회사 Battery and method for producing the same
KR101893608B1 (en) * 2010-08-06 2018-08-30 가부시키가이샤 무라타 세이사쿠쇼 Battery and method for producing the same

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