JP2001126678A - Laminate polymer electrolyte battery - Google Patents

Laminate polymer electrolyte battery

Info

Publication number
JP2001126678A
JP2001126678A JP30622099A JP30622099A JP2001126678A JP 2001126678 A JP2001126678 A JP 2001126678A JP 30622099 A JP30622099 A JP 30622099A JP 30622099 A JP30622099 A JP 30622099A JP 2001126678 A JP2001126678 A JP 2001126678A
Authority
JP
Japan
Prior art keywords
negative electrode
polymer electrolyte
positive electrode
heat
resin film
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.)
Withdrawn
Application number
JP30622099A
Other languages
Japanese (ja)
Inventor
Hiroshi Yamamoto
宏 山本
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.)
Maxell Holdings Ltd
Original Assignee
Hitachi Maxell Ltd
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 Hitachi Maxell Ltd filed Critical Hitachi Maxell Ltd
Priority to JP30622099A priority Critical patent/JP2001126678A/en
Publication of JP2001126678A publication Critical patent/JP2001126678A/en
Withdrawn legal-status Critical Current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

Landscapes

  • Sealing Battery Cases Or Jackets (AREA)

Abstract

PROBLEM TO BE SOLVED: To provide a laminate polymer electrolyte battery with high reliability that prevents the short circuit owing to the modifying of the slanting portion between the part of the enclosure material close to the laminate electrode body to the sealing part of the enclosure material when pressing the laminate electrode body through the enclosure material for reduced sealing. SOLUTION: A laminate electrode body obtained by interposing a polymer electrolyte between the positive and negative electrodes is sealed with an enclosure material consisting of a protective film, metal film, and heat-fused resin film. A heat-fused resin film having the same composition as that of the enclosure material is laid on the connection region between the positive lead and terminal and its near region, and the connection region between the negative lead and terminal and its near region, so that there is prevented the short circuit owing to the modifying of the slanting portion of the enclosure material obtained by the reduced press sealing.

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、積層形ポリマー電
解質電池に関し、さらに詳しくは、特に携帯用電子機
器、電気自動車、ロードレベリングなどの電源として使
用するのに適した積層形ポリマー電解質電池に関する。
BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a stacked polymer electrolyte battery, and more particularly, to a stacked polymer electrolyte battery suitable for use as a power source for portable electronic devices, electric vehicles, road leveling, and the like.

【0002】[0002]

【従来の技術】ポリマー電解質電池では、電極および電
解質をシート状にすることができ、それによって、A4
版、B5版などの大面積でしかも薄形の電池の作製が可
能になり、各種薄形製品への適用が可能になるため、電
池の使用範囲が大きく広がっている。特にポリマー電解
質を用いた電池は、耐漏液性を含めた安全性、貯蔵性が
優れており、しかも薄く、フレキシブルであることか
ら、機器の形状に合わせた電池を設計できるという、今
までの電池にない特徴を持っている。
2. Description of the Related Art In a polymer electrolyte battery, the electrodes and the electrolyte can be made into a sheet shape, whereby A4
It is possible to manufacture a large-sized and thin battery such as a plate and a B5 plate, and it is possible to apply the battery to various thin products. Therefore, the range of use of the battery is greatly expanded. In particular, batteries using polymer electrolytes have excellent safety and storage properties, including liquid leakage resistance, and are thin and flexible, so that batteries that match the shape of equipment can be designed to date. Has features not found in

【0003】このポリマー電解質電池は、通常、アルミ
ニウム箔などの金属箔を芯材にし、内面側に接着層とな
る熱融着性樹脂フィルムを配置したラミネートフィルム
を外装材に用い、得ようとする電気容量に応じて、複数
枚のシート状電極と複数枚のシート状のポリマー電解質
電池とを積層した電極積層体を外装材で外装することに
よって、薄いシート形電池に仕上げられることが行われ
ている。
[0003] This polymer electrolyte battery is usually obtained by using, as an exterior material, a laminate film in which a metal foil such as an aluminum foil is used as a core material and a heat-fusible resin film serving as an adhesive layer is disposed on the inner surface side. Depending on the electric capacity, a thin sheet-type battery is performed by packaging an electrode laminate obtained by laminating a plurality of sheet-like electrodes and a plurality of sheet-like polymer electrolyte batteries with an exterior material. I have.

【0004】そして、上記電極積層体を金属箔を芯材と
するラミネートフィルムからなる外装材により封止する
場合、通常、電極積層体より大きい外装材を2枚用い、
それを電極積層体の上下に配置し、外装材同士の接合部
分を加熱して、外装材の接着層を構成する熱融着性樹脂
フィルムの樹脂同士を接着させて封止するか、あるい
は、上記外装材を袋状にしておき、その内部に電極積層
体を収容した後、その開口部を加熱して外装材の接着層
を構成する熱融着性樹脂フィルムの樹脂同士を接着させ
て封止する方法が採用されている。つまり、封止に際し
ては、接着層が主として働き、外気との遮断に際しては
金属箔と接着層とが主として働き、電極のリード部の取
り出しは、上記外装材の封止部分より取り出されること
になる。
[0004] When the electrode laminate is sealed with a packaging material composed of a laminate film having a metal foil as a core material, usually, two packaging materials larger than the electrode laminate are used.
It is placed above and below the electrode laminate, and the joint between the exterior materials is heated, and the resin of the heat-fusible resin film constituting the adhesive layer of the exterior material is bonded and sealed, or After the outer packaging material is formed in a bag shape and the electrode laminate is accommodated therein, the opening thereof is heated to bond the resin of the heat-fusible resin film constituting the adhesive layer of the outer packaging material and seal it. The method of stopping is adopted. That is, at the time of sealing, the adhesive layer mainly functions, and at the time of shielding from outside air, the metal foil and the adhesive layer mainly function, and the lead portion of the electrode is taken out from the sealing portion of the exterior material. .

【0005】ところが、上記金属箔を芯材とするラミネ
ートフィルムからなる外装材で電極積層体を封止した場
合、電極のリード部と外装材の金属箔とが接触し、その
金属箔を介して正負極間の短絡が生じるという問題があ
った。
However, when the electrode laminate is sealed with a package made of a laminate film having the above-mentioned metal foil as a core material, the lead portion of the electrode and the metal foil of the package come into contact with each other, and the metal foil passes through the metal foil. There is a problem that a short circuit occurs between the positive and negative electrodes.

【0006】すなわち、電極のリード部は金属で構成さ
れているため、外装材としてのラミネートフィルムの接
着層の構成樹脂との接着は必ずしも良好でなく、通常、
外装材の接着層の構成樹脂同士の接着より長い時間また
は高い温度が必要である。そのため、外装材の接着層の
構成樹脂が溶融しすぎて、芯材の金属箔がむき出しの状
態になり、それが電極のリード部と接触し、その金属箔
を介して正極と負極とが短絡することになる。
That is, since the lead portion of the electrode is made of metal, the adhesion of the adhesive layer of the laminate film as the exterior material to the constituent resin is not always good.
It requires a longer time or a higher temperature than the bonding between the constituent resins of the adhesive layer of the exterior material. As a result, the constituent resin of the adhesive layer of the exterior material is excessively melted, and the metal foil of the core material is exposed, which comes into contact with the lead of the electrode, and the positive electrode and the negative electrode are short-circuited via the metal foil. Will do.

【0007】また、外装材による封止は、封止後の積層
形ポリマー電解質電池の外観を向上させることもあって
減圧(真空)封止を行っているが、減圧封止により、外
装材の電極積層体の本体部分が配置する部分から外装材
の封止部に至る傾斜部分が変形し、その結果、正極のリ
ード部と正極端子との接続部の電池内部側の端部および
負極のリード部と負極端子との接続部の電池内部側の端
部が外装材のラミネートフィルムの接着層を構成する熱
融着性樹脂フィルムを突き破り、短絡を引き起こすとい
う問題があった。
[0007] In addition, in order to improve the appearance of the laminated polymer electrolyte battery after sealing, decompression (vacuum) sealing is performed in order to improve the appearance of the laminated polymer electrolyte battery. The inclined portion from the portion where the main body portion of the electrode laminate is disposed to the sealing portion of the exterior material is deformed, and as a result, the inside of the battery at the end of the connection between the positive electrode lead and the positive electrode terminal and the negative electrode lead There is a problem that the end on the battery inner side of the connection portion between the portion and the negative electrode terminal breaks through the heat-fusible resin film constituting the adhesive layer of the laminate film of the exterior material, causing a short circuit.

【0008】[0008]

【発明が解決しようとする課題】本発明は、上記のよう
な従来技術における問題点を解決し、外装材で電極積層
体を減圧封止したときの傾斜部分の変形によって生じる
短絡を防止し、信頼性の高い積層形ポリマー電解質電池
を提供することを目的とする。
SUMMARY OF THE INVENTION The present invention solves the above-described problems in the prior art, and prevents a short circuit caused by deformation of an inclined portion when an electrode laminate is sealed under reduced pressure with a packaging material. An object of the present invention is to provide a highly reliable laminated polymer electrolyte battery.

【0009】[0009]

【課題を解決するための手段】本発明は、正極と負極と
をそれらの間にポリマー電解質を介在させて積層した電
極積層体を、保護フィルムと金属箔と熱融着性樹脂フィ
ルムとのラミネートフィルムからなる外装材で封止する
構造の積層形ポリマー電解質電池において、正極のリー
ド部と正極端子との接続部およびその近傍ならびに負極
のリード部と負極端子との接続部およびその近傍に上記
外装材を構成するラミネートフィルムの熱融着性樹脂フ
ィルムと同一材質の熱融着性樹脂フィルムを配設するこ
とによって、外装材の減圧封止による傾斜部分の変形に
よって生じる短絡の発生を防止することにより、上記課
題を解決したものである。
According to the present invention, there is provided an electrode laminate comprising a positive electrode and a negative electrode laminated with a polymer electrolyte interposed therebetween, by laminating a protective film, a metal foil and a heat-fusible resin film. In a laminated polymer electrolyte battery having a structure sealed with a film-made outer material, the outer package is provided at a connection portion between a lead portion of a positive electrode and a positive electrode terminal and in the vicinity thereof, and at a connection portion between a lead portion of a negative electrode and a negative electrode terminal and in the vicinity thereof. By disposing a heat-fusible resin film of the same material as the heat-fusible resin film of the laminated film that constitutes the material, it is possible to prevent the occurrence of a short circuit caused by the deformation of the inclined portion due to the reduced pressure sealing of the exterior material. Thus, the above problem has been solved.

【0010】すなわち、本発明では、真空封止により外
装材の傾斜部分に変形が生じた場合でも、正極のリード
部と正極端子との接続部の近傍ならびに負極のリード部
と負極端子との接続部の近傍に配設した熱融着性樹脂フ
ィルムにより、上記正極のリード部と正極端子との接続
部の電池内部側の端部や負極のリード部と負極端子との
接続部の電池内部側の端部が外装材を構成するラミネー
トフィルムの熱融着性樹脂フィルムを突き破って短絡を
引き起こすのを防止することができるようにしたのであ
る。
That is, according to the present invention, even when the inclined portion of the exterior material is deformed by vacuum sealing, the vicinity of the connection portion between the positive electrode lead portion and the positive electrode terminal and the connection between the negative electrode lead portion and the negative electrode terminal are reduced. The end of the connection between the positive electrode lead and the positive electrode terminal on the battery inside side and the connection between the negative electrode lead and the negative electrode terminal inside the battery by the heat-fusible resin film disposed in the vicinity of the Is prevented from breaking through the heat-fusible resin film of the laminate film constituting the exterior material and causing a short circuit.

【0011】[0011]

【発明の実施の形態】本発明において、正極は正極集電
体の少なくとも一方の面に正極合剤層を形成することに
よって作製され、通常、そのリード部は正極の作製時に
正極集電体の一部に正極合剤層を形成せずに正極集電体
の露出部分を残しておくことによって設けられる。ただ
し、正極のリード部は上記以外の手段によって正極に設
けてもよい。上記正極集電体や正極合剤は公知の構成の
ものでもよく、例えば、正極集電体としてはアルミニウ
ム箔が特に好適に用いられる。
DESCRIPTION OF THE PREFERRED EMBODIMENTS In the present invention, a positive electrode is manufactured by forming a positive electrode mixture layer on at least one surface of a positive electrode current collector. It is provided by leaving the exposed portion of the positive electrode current collector without forming the positive electrode mixture layer in a part. However, the lead portion of the positive electrode may be provided on the positive electrode by means other than the above. The positive electrode current collector and the positive electrode mixture may have a known structure. For example, an aluminum foil is particularly suitably used as the positive electrode current collector.

【0012】また、負極は負極集電体の少なくとも一方
の面に負極合剤層を形成することに作製され、通常、そ
のリード部は負極の作製時に負極集電体の一部に負極合
剤層を形成せずに負極集電体の露出部分を残すことによ
って設けられる。ただし、負極のリード部は上記以外の
手段によって設けてもよい。上記負極集電体や負極合剤
層は公知の構成のものでもよく、例えば、負極集電体と
しては銅箔が特に好適に用いられる。
The negative electrode is produced by forming a negative electrode mixture layer on at least one surface of the negative electrode current collector. Usually, the lead portion is formed on a part of the negative electrode current collector when the negative electrode is produced. It is provided by leaving an exposed portion of the negative electrode current collector without forming a layer. However, the lead portion of the negative electrode may be provided by means other than the above. The negative electrode current collector and the negative electrode mixture layer may have a known configuration. For example, a copper foil is particularly preferably used as the negative electrode current collector.

【0013】ポリマー電解質も、従来構成と同様のもの
を用いることができ、例えば、上記ポリマー電解質を構
成するための電解液としては、例えばジメチルカーボネ
ート、ジエチルカーボネート、メチルエチルカーボネー
ト、プロピオン酸メチル、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、エチレングリコールサルファイト、1,2
−ジメトキシエタン、1,3−ジオキソラン、テトラヒ
ドロフラン、2−メチル−テトラヒドロフラン、ジエチ
ルエーテルなどの有機溶媒に、例えばLiClO4 、L
iPF6 、LiBF4 、LiAsF6 、LiCF3 SO
3 、LiC4 9 SO3 、LiCF3 CO2 、Li2
2 4 (SO3 2 、LiN(CF3 SO2 2 、Li
C(CF 3 SO2 3 、LiCn 2n+1SO3 (n≧
2)、LiN(RfOSO2 2 〔ここではRfはフル
オロアルキル基〕などの無機イオン塩を溶解させること
によって調製したものが使用され、また、上記電解液を
ゲル化させるためのゲル化成分としては、例えばポリフ
ッ化ビニリデン、ポリエチレンオキサイド、ポリアクリ
ロニトリル、フッ化ビニリデン−六フッ化プロピレン共
重合体などのように直鎖状のポリマーを加熱することに
より電解液に溶解させた後、冷却することによって電解
液をゲル化させるポリマーや、例えばジペンタエリスリ
トールヘキサアクリレートなどの活性光線(例えば紫外
線、電子線など)で重合可能な二重結合を一分子あたり
2個以上含みモノマーまたはプレポリマーを主成分とす
る架橋性組成物などが用いられる。
[0013] The polymer electrolyte is the same as the conventional one.
For example, the above-mentioned polymer electrolyte can be used.
As an electrolytic solution for forming, for example, dimethyl carbonate
, Diethyl carbonate, methyl ethyl carbonate
G, methyl propionate, ethylene carbonate, pro
Pyrene carbonate, butylene carbonate, γ-butyl
Lolactone, ethylene glycol sulfite, 1,2
-Dimethoxyethane, 1,3-dioxolan, tetrahi
Drofuran, 2-methyl-tetrahydrofuran, diethyl
Organic solvents such as toluene, for example, LiClOFour, L
iPF6, LiBFFour, LiAsF6, LiCFThreeSO
Three, LiCFourF9SOThree, LiCFThreeCOTwo, LiTwoC
TwoFFour(SOThree)Two, LiN (CFThreeSOTwo)Two, Li
C (CF ThreeSOTwo)Three, LiCnF2n + 1SOThree(N ≧
2), LiN (RfOSOTwo)Two[Rf is full here
Dissolving inorganic ion salts such as
Is used, and the above electrolyte is
As a gelling component for gelling, for example,
Vinylidene fluoride, polyethylene oxide, polyacrylic
Ronitrile, vinylidene fluoride-propylene hexafluoride
Heating linear polymers such as polymers
After dissolving in more electrolytic solution, cooling
Polymers that gel liquids, such as dipentaerythri
Actinic rays such as tall hexaacrylate (eg, ultraviolet
Double bonds polymerizable by electron beam, electron beam, etc.) per molecule
Containing two or more monomers and predominantly monomer or prepolymer
A crosslinkable composition or the like is used.

【0014】本発明において、電極積層体の封止のため
に用いる外装材は、保護フィルムと金属箔と熱融着性樹
脂フィルムとのラミネートフィルムからなり、上記保護
フィルムは電池外部側に配置されるもので、例えば、ナ
イロンフィルム、ポリエステルフィルムなどが用いら
れ、その内部側に位置するアルミニウム箔などの金属箔
を保護し、金属箔が他のものとの接触により損傷を受け
たり、金属箔(特にアルミニウム箔)が外気との接触に
より腐食するのを防止する。上記金属箔としては、特に
その材質が限定されるものではないが、通常、延展性に
富むアルミニウム箔が用いられ、この金属箔は水分や空
気の透過を防止する役割を担っている。また、熱融着性
樹脂フィルムは、接着層としての役割を果たすもので、
例えば、変性ポリオレフィンフィルムなどが用いられ
る。
In the present invention, the exterior material used for sealing the electrode laminate comprises a laminate film of a protective film, a metal foil, and a heat-fusible resin film, and the protective film is disposed outside the battery. For example, a nylon film, a polyester film, or the like is used to protect a metal foil such as an aluminum foil located on the inner side thereof. Especially, aluminum foil) is prevented from being corroded by contact with the outside air. The metal foil is not particularly limited in its material, but usually, an aluminum foil having a high spreadability is used, and this metal foil has a role of preventing permeation of moisture and air. In addition, the heat-fusible resin film plays a role as an adhesive layer,
For example, a modified polyolefin film is used.

【0015】そして、正極のリード部と正極端子との接
続部およびその近傍ならびに負極のリード部と負極端子
との接続部およびその近傍に配設する熱融着性樹脂フィ
ルムとしては、外装材の接着層となる熱融着性樹脂フィ
ルムとの接着性を考慮として外装材の熱融着性樹脂フィ
ルムと同一材質のものを用いるので、上記外装材の熱融
着性樹脂フィルムとして例示のものをいずれも用いるこ
とができるが、この熱融着性樹脂フィルムとしても変性
ポリオレフィンフィルムが特に好適に用いられる。この
熱融着性樹脂フィルムの厚みとしては、特に限定される
ものではないが、20〜100μm程度のものが好まし
い。つまり、上記熱融着性樹脂フィルムの厚みが上記よ
り薄い場合は、充分な効果が得られず、また、熱融着性
樹脂フィルムの厚みが上記より厚くなると、熱融着時に
電池外部に熱融着性樹脂フィルムがはみ出し外観を低下
させるおそれがある。
The heat-fusible resin film disposed at and near the connection between the lead portion of the positive electrode and the positive electrode terminal and near the connection between the lead portion of the negative electrode and the negative electrode terminal, and Since the same material as the heat-fusible resin film of the exterior material is used in consideration of the adhesiveness with the heat-fusible resin film to be the adhesive layer, the heat-fusible resin film of the above-mentioned exterior material is exemplified. Although any of them can be used, a modified polyolefin film is particularly preferably used as the heat-fusible resin film. The thickness of the heat-fusible resin film is not particularly limited, but is preferably about 20 to 100 μm. In other words, when the thickness of the heat-fusible resin film is smaller than the above, a sufficient effect cannot be obtained. The fusible resin film may protrude and reduce the appearance.

【0016】上記熱融着性樹脂フィルムの正極のリード
部と正極端子との接続部および負極のリード部と負極端
子との接続部に配設する部分は上記接続部における外装
材の熱融着性樹脂フィルムの不足分を補って電池内部の
密封性を保つためのものであり、また、その接続部の近
傍に配置する部分は前記のように正極のリード部と正極
端子との接続部の電池内部側の端部や負極のリード部と
負極端子との接続部の電池内部側の端部が外装材の熱融
着性樹脂フィルムを突き破って短絡を引き起こすのを防
止するものであるから、上記接続部の近傍に配設する熱
融着性樹脂フィルムとしては、正極側では上記のように
正極のリード部と正極端子との接続部の電池内部側の端
部にまで達していればよいが、それを越えてさらに電池
内部側まで達していてもよい。また、負極側では、上記
熱融着性樹脂フィルムは、負極のリード部と負極端子と
の接続部の電池内部側の端部にまで達していればよい
が、それを越えてさらに電池内部側まで達していてもよ
い。
The portion provided at the connection between the positive electrode lead and the positive electrode terminal and the connection between the negative electrode lead and the negative electrode terminal of the heat-fusible resin film is formed by heat-sealing the exterior material at the connection. It is intended to compensate for the shortage of the conductive resin film and to maintain the sealing property inside the battery, and the portion disposed near the connection portion is the connection portion between the lead portion of the positive electrode and the positive electrode terminal as described above. Since the inside end of the battery and the inside end of the battery at the connection between the lead portion of the negative electrode and the negative terminal are prevented from breaking through the heat-fusible resin film of the exterior material and causing a short circuit, As the heat-fusible resin film disposed in the vicinity of the connection portion, the positive electrode side may reach the end of the connection portion between the lead portion of the positive electrode and the positive electrode terminal on the inside of the battery as described above. But beyond that, it reaches the inside of the battery It may be. On the negative electrode side, the heat-fusible resin film only needs to reach the inside of the battery at the connection between the lead portion of the negative electrode and the negative electrode terminal. May have been reached.

【0017】そして、この熱融着性樹脂フィルムの配設
にあたっては、あらかじめ外装材の熱融着性樹脂フィル
ムに貼り付けておくことが適しており、それによって、
生産性を向上させることができる。また、この熱融着性
樹脂フィルムの配設によって従来正極端子や負極端子に
あらかじめ取り付けていた封止材が不要になり、この面
でも生産性が向上する。
When disposing the heat-fusible resin film, it is suitable to attach the heat-fusible resin film to the heat-fusible resin film of the exterior material in advance.
Productivity can be improved. Further, the provision of the heat-fusible resin film eliminates the need for a sealing material previously attached to the positive electrode terminal or the negative electrode terminal in the past, and thus improves productivity.

【0018】[0018]

【実施例】つぎに、実施例を挙げて本発明をより具体的
に説明する。ただし、本発明は実施例に例示のもののみ
に限定されることはない。
Next, the present invention will be described more specifically with reference to examples. However, the present invention is not limited to only those illustrated in the embodiments.

【0019】実施例1 まず、この実施例1において用いる正極および負極の作
製、ゲル化成分含有電解液の調製について先に説明す
る。
Example 1 First, the preparation of a positive electrode and a negative electrode used in Example 1 and the preparation of an electrolyte containing a gelling component will be described first.

【0020】正極の作製:正極活物質であるLiCoO
2 80重量部、導電助剤であるアセチレンブラック5重
量部、バインダーであるポリフッ化ビニリデン5重量部
とをN−メチルピロリドンを溶媒として均一になるよう
に混合し、正極合剤含有ペーストを調製した。この正極
合剤含有ペーストを厚さ20μmのアルミニウム箔から
なる正極集電体の両面に塗布し、乾燥した後、カレンダ
ー処理を行って、全厚が130μmになるように正極合
剤層の厚みを調整し、正極合剤層形成部分の面積が70
mm×40mmになるように切断して正極を作製した。
ただし、上記正極の作製にあたっては、アルミニウム箔
の長辺方向の端部に正極合剤含有ペーストを塗布せず
に、幅7mm、長さ20mmのアルミニウム箔の露出部
分を残し、そのアルミニウム箔の露出部分を正極端子な
どとの接続のためのリード部とした。この正極の断面図
を図1に模式的に示す。図1に示すように、この正極1
は正極集電体1aの両面に正極合剤層1bを形成するこ
とによって作製され、そのリード部1cは上記正極集電
体1aを構成するアルミニウム箔の一部に正極合剤含有
ペーストを塗布せず、正極集電体1aを構成するアルミ
ニウム箔を露出させることによって構成されている。
Preparation of positive electrode: LiCoO as positive electrode active material
2 80 parts by weight of acetylene black 5 parts by weight of conductive additive, a polyvinylidene fluoride 5 parts by weight of the N- methylpyrrolidone as a binder and mixed uniformly as a solvent, to prepare a positive electrode mixture-containing paste . This positive electrode mixture-containing paste is applied to both surfaces of a positive electrode current collector made of an aluminum foil having a thickness of 20 μm, dried, and subjected to a calendering process to reduce the thickness of the positive electrode mixture layer so that the total thickness becomes 130 μm. The area of the positive electrode mixture layer forming part was adjusted to 70
A positive electrode was prepared by cutting the sample to a size of mm × 40 mm.
However, in preparing the positive electrode, the positive electrode mixture-containing paste was not applied to the end of the aluminum foil in the long side direction, and the exposed portion of the aluminum foil having a width of 7 mm and a length of 20 mm was left. The portion was used as a lead portion for connection to a positive terminal or the like. FIG. 1 schematically shows a cross-sectional view of this positive electrode. As shown in FIG.
Is formed by forming a positive electrode mixture layer 1b on both sides of a positive electrode current collector 1a, and its lead portion 1c is formed by applying a positive electrode mixture-containing paste to a part of the aluminum foil constituting the positive electrode current collector 1a. Instead, it is constituted by exposing the aluminum foil constituting the positive electrode current collector 1a.

【0021】負極Aの作製:負極活物質である黒鉛90
重量部とカーボトロンP(商品名、呉羽化学工業社製の
低結晶カーボン)を8重量部とバインダーであるポリフ
ッ化ビニリデン15重量部とをN−メチルピロリドンを
溶媒として均一になるように混合して負極合剤含有ペー
ストを調製し、厚さ10μmの銅箔からなる負極集電体
の両面に塗布し、乾燥した後、カレンダー処理を行って
全厚が130μmになるように負極合剤層の厚みを調整
し、負極合剤層形成部分の面積が72mm×42mmに
なるように切断して負極を作製した。また、この負極の
作製にあたっては、銅箔の長辺方向の端部に負極合剤含
有ペーストを塗布せず、幅7mm、長さ20mmの銅箔
の露出部分を残し、その銅箔の露出部分を負極端子など
との接続のためのリード部とした。このようにして作製
した負極Aは、負極合剤層が負極集電体の両面に形成さ
れた、いわゆる両面塗布負極と呼ばれるものである。こ
の負極Aの断面図を図2に模式的に示す。図2に示すよ
うに、負極Aは負極集電体2aの両面に負極合剤層2b
を形成することによって作製され、そのリード部2cは
上記負極集電体2aを構成する銅箔の一部に負極合剤含
有ペーストを塗布せず、銅箔を露出させて構成されてい
る。なお、図示にあたっては、この負極Aおよび後述の
負極Bとも同一の参照符号2を付して示す。
Preparation of Negative Electrode A: Graphite 90 as negative electrode active material
Parts by weight, 8 parts by weight of CARBOTRON P (trade name, low crystalline carbon manufactured by Kureha Chemical Industry Co., Ltd.) and 15 parts by weight of polyvinylidene fluoride as a binder are mixed uniformly using N-methylpyrrolidone as a solvent. A negative electrode mixture-containing paste is prepared, applied to both surfaces of a negative electrode current collector made of a copper foil having a thickness of 10 μm, dried, and then subjected to a calendering process so that the total thickness of the negative electrode mixture layer is 130 μm. Was adjusted and cut so that the area of the negative electrode mixture layer forming portion was 72 mm × 42 mm, to produce a negative electrode. Also, in producing the negative electrode, the negative electrode mixture-containing paste was not applied to the end of the copper foil in the long side direction, and the exposed portion of the copper foil having a width of 7 mm and a length of 20 mm was left. Is a lead portion for connection with a negative electrode terminal or the like. The negative electrode A thus manufactured is a so-called double-sided coated negative electrode in which a negative electrode mixture layer is formed on both surfaces of a negative electrode current collector. FIG. 2 schematically shows a cross-sectional view of the negative electrode A. As shown in FIG. 2, the negative electrode A has a negative electrode mixture layer 2b on both surfaces of a negative electrode current collector 2a.
The lead portion 2c is formed by exposing the copper foil without applying the negative electrode mixture-containing paste on a part of the copper foil constituting the negative electrode current collector 2a. In the drawings, the negative electrode A and a negative electrode B described later are denoted by the same reference numeral 2.

【0022】負極Bの作製:上記負極Aの場合と同様の
負極合剤含有ペーストを厚さ10μmの銅箔からなる負
極集電体の片面に塗布し、乾燥した後、カレンダー処理
を行って全厚が70μmになるように負極合剤層の厚み
を調整し、負極合剤層の形成部分の面積が72mm×4
2mmになるように切断して負極Bを作製した。この負
極Bの作製にあたっても、銅箔の長辺方向の端部に負極
合剤含有ペーストを塗布せず、幅7mm、長さ20mm
の銅箔の露出部分を残し、その銅箔の露出部分を負極端
子などとの接続のためのリード部とした。このようにし
て作製された負極Bは、負極合剤層が負極集電体の片面
のみに形成された、いわゆる片面塗布負極と呼ばれるも
のである。この負極Bの断面図を図3に模式的に示す。
図3に示すように、この負極Bは負極集電体2aの片面
のみに負極合剤層2bを形成することによって作製され
ている。
Preparation of Negative Electrode B: The same negative electrode mixture-containing paste as in the case of the above-mentioned negative electrode A was applied to one side of a negative electrode current collector made of a copper foil having a thickness of 10 μm, dried, and subjected to a calendering treatment. The thickness of the negative electrode mixture layer was adjusted so that the thickness became 70 μm, and the area of the portion where the negative electrode mixture layer was formed was 72 mm × 4.
This was cut to 2 mm to produce a negative electrode B. In producing the negative electrode B, the paste containing the negative electrode mixture was not applied to the end in the long side direction of the copper foil, and the width was 7 mm and the length was 20 mm.
The exposed portion of the copper foil was left, and the exposed portion of the copper foil was used as a lead portion for connection with a negative electrode terminal or the like. The negative electrode B thus produced is a so-called single-sided coated negative electrode in which the negative electrode mixture layer is formed only on one side of the negative electrode current collector. FIG. 3 schematically shows a cross-sectional view of the negative electrode B.
As shown in FIG. 3, the negative electrode B is manufactured by forming the negative electrode mixture layer 2b on only one surface of the negative electrode current collector 2a.

【0023】ゲル化成分含有電解液の調製:プロピレン
カーボネートとエチレンカーボネートとの体積比1:1
の混合溶媒にLiPF6 を1.22mol/l溶解させ
ることによって調製した電解液に開始剤として2,4,
6−トリメチルベンゾイルジフェニルフォスフィンオキ
サイド〔商品名:ルシリンTPO、ビーエーエスエフジ
ャパン(株)製〕をあらかじめモノマー成分に対して2
重量%加えて溶解しておき、そこにジペンタエリスリト
ールヘキサアクリレートを使用開始10分前に濃度が6
重量%になるように加えて混合し、ゲル化成分を含有す
る電解液を調製した。このゲル化成分を含有する電解液
を上記標題のように「ゲル化成分含有電解液」と簡略化
して表現する。
Preparation of electrolyte solution containing gelling component: 1: 1 volume ratio of propylene carbonate to ethylene carbonate
As an initiator, 2,4,4 was dissolved in an electrolyte prepared by dissolving 1.22 mol / l of LiPF 6 in a mixed solvent of
6-trimethylbenzoyldiphenylphosphine oxide (trade name: Lucirin TPO, manufactured by BSF Japan Co., Ltd.)
Wt% and dissolved therein, and dipentaerythritol hexaacrylate was added to the mixture at a concentration of 6 minutes before the start of use.
The mixture was added and mixed so as to obtain a weight percent, thereby preparing an electrolytic solution containing a gelling component. The electrolytic solution containing the gelling component is simply expressed as “gelling component-containing electrolytic solution” as described above.

【0024】上記のように作製した正極をポリマー電解
質の支持体となる不織布で包んで、正極と支持体とを一
体化しておき、その全体にゲル化成分含有電解液を含浸
させ、ゲル化して、ポリマー電解質保持正極ユニットを
得た。負極は不織布で包むことなく、ゲル化成分含有電
解液を含浸させ、ゲル化して、ポリマー電解質保持負極
を得た。それらの作製方法の詳細を次に示す。
The positive electrode prepared as described above is wrapped with a nonwoven fabric serving as a support for the polymer electrolyte, and the positive electrode and the support are integrated, and the whole is impregnated with a gelling component-containing electrolytic solution and gelled. Thus, a positive electrode unit holding a polymer electrolyte was obtained. The negative electrode was impregnated with a gelling component-containing electrolytic solution without being wrapped with a nonwoven fabric, and gelled to obtain a polymer electrolyte-holding negative electrode. The details of the manufacturing method are described below.

【0025】ポリマー電解質保持正極の作製:支持体と
しては、厚さ30μm、坪量12g/m2 のポリブチレ
ンテレフタレート不織布〔NKK社製、MB1230
(商品名)〕を用いた。
Preparation of Polymer Electrolyte-Supported Positive Electrode: As a support, a polybutylene terephthalate nonwoven fabric having a thickness of 30 μm and a basis weight of 12 g / m 2 [MB1230, manufactured by NKK Corporation]
(Trade name)] was used.

【0026】そして、正極の正極合剤層形成部分とリー
ド部とにまたがるようにして、厚さ50μm、幅3mm
のポリイミドテープをその両面から貼着し、短絡の防止
および端子の強度保持と図った。また、リード部の正極
端子との接続に用いる部分のすべての表面を、熱により
接着面の粘着性が失われる熱剥離テープで被覆した後、
この正極を上記ポリブチレンテレフタレート不織布の長
さ方向の中央部より左側の部分に載置し、右側の部分を
折り返して正極を覆った後、その幅方向の両側部を熱融
着器〔商品名:ポリシーラー、富士インパルス(株)
製〕でシールして支持体としてのポリブチレンテレフタ
レート不織布を袋状にし、両者を密接させて正極と支持
体とを一体化した。この正極と支持体とを一体化した正
極ユニットを前記ゲル化成分含有電解液に減圧下で1分
間浸漬して正極ユニットにゲル化成分含有電解液を含浸
させた後、ポリエチレン製の袋に入れて密閉した。つぎ
に、そのポリエチレン製袋の両面から、フュージョンU
Vシステムズ・ジャパン(株)製の紫外線照射装置を用
いて、紫外線を1W/cm2 の照度で10秒間照射し、
電解液中のモノマー成分を重合させるとともに、電解液
をゲル化してゲル状ポリマー電解質とした。このポリマ
ー電解質を保持させた正極を袋から取り出し、そのリー
ド部の正極端子との接続に用いる部分に150℃の熱風
を吹き付けることによって熱剥離テープを該部分から剥
がし、ポリマー電解質保持正極を得た。
Then, the positive electrode is formed to have a thickness of 50 μm and a width of 3 mm so as to extend over the positive electrode mixture layer forming portion of the positive electrode and the lead portion.
Was adhered from both sides to prevent short circuit and maintain the strength of the terminals. Also, after covering the entire surface of the portion of the lead portion used for connection with the positive electrode terminal with a heat release tape that loses the adhesiveness of the adhesive surface due to heat,
The positive electrode is placed on the left side of the center of the polybutylene terephthalate nonwoven fabric in the longitudinal direction, and the right side is folded back to cover the positive electrode. : Policyr, Fuji Impulse Co., Ltd.
And a bag made of a polybutylene terephthalate nonwoven fabric as a support, and the two were brought into close contact to integrate the positive electrode and the support. The positive electrode unit in which the positive electrode and the support are integrated is immersed in the gelling component-containing electrolyte for 1 minute under reduced pressure to impregnate the positive electrode unit with the gelling component-containing electrolyte, and then put in a polyethylene bag. And sealed. Next, from both sides of the polyethylene bag, Fusion U
Using an ultraviolet irradiator manufactured by V Systems Japan Co., Ltd., irradiate ultraviolet rays at an illuminance of 1 W / cm 2 for 10 seconds,
The monomer component in the electrolytic solution was polymerized, and the electrolytic solution was gelled to obtain a gel polymer electrolyte. The positive electrode holding the polymer electrolyte was taken out of the bag, and the thermal release tape was peeled off from the part by blowing hot air at 150 ° C. onto the part of the lead part used for connection with the positive electrode terminal, thereby obtaining a positive electrode holding the polymer electrolyte. .

【0027】ポリマー電解質保持負極Aの作製:上記の
ように作製した負極Aの負極合剤層形成部分とリード部
とにまたがるようにして、厚さ50μm、幅3mmのポ
リイミドテープをその両面から貼着し、短絡の防止およ
び端子の強度保持を図った。また、リード部の負極端子
との接続に用いる部分のすべての表面を、熱により接着
面の粘着性が失われる熱剥離テープで被覆した後、この
負極Aを前記ゲル化成分含有電解液に減圧下で1分間浸
漬して、ゲル化成分含有電解液を含浸させた後、ポリエ
チレン製の袋に入れて密閉した。つぎに、ポリエチレン
製の袋の両面から、フュージョンUVシステムズ・ジャ
パン(株)製の紫外線照射装置を用いて、紫外線を1W
/cm2 の照度で10秒間照射し、電解液中のモノマー
成分を重合させるとともに、電解液をゲル化してゲル状
ポリマー電解質とした。このゲル状ポリマー電解質を保
持させた負極Aを袋から取り出し、そのリード部の負極
端子との接続に用いる部分に150℃の熱風を吹き付け
ることによって熱剥離テープを該部分から剥がし、ポリ
マー電解質保持負極Aを得た。
Preparation of polymer electrolyte-holding negative electrode A: A polyimide tape having a thickness of 50 μm and a width of 3 mm was attached to both sides of the negative electrode A prepared as described above so as to extend over the negative electrode mixture layer forming portion and the lead portion. To prevent short circuits and maintain the strength of the terminals. After covering the entire surface of the portion of the lead portion used for connection with the negative electrode terminal with a heat release tape that loses the adhesiveness of the adhesive surface due to heat, the negative electrode A was decompressed into the gelled component-containing electrolytic solution. After immersion for 1 minute in the lower part to impregnate the electrolytic solution containing the gelling component, the resultant was put in a polyethylene bag and sealed. Next, ultraviolet light was applied to both sides of the polyethylene bag at a rate of 1 W using an ultraviolet irradiation device manufactured by Fusion UV Systems Japan Co., Ltd.
Irradiation was performed for 10 seconds at an illuminance of / cm 2 to polymerize the monomer components in the electrolytic solution and gel the electrolytic solution to obtain a gel polymer electrolyte. The negative electrode A holding the gelled polymer electrolyte is taken out of the bag, and hot air of 150 ° C. is blown to a portion of the lead portion used for connection with the negative electrode terminal, thereby peeling off the thermal release tape from the portion. A was obtained.

【0028】ポリマー電解質保持負極Bの作製:上記の
ように作製した負極Bの負極合剤層形成部分とリード部
とにまたがるようにして、厚さ50μm、幅3mmのポ
リイミドテープをその両面から貼着し、短絡の防止およ
び端子の強度保持を図った。また、リード部の負極端子
との接続に用いる部分のすべての表面を、熱により接着
面の粘着性が失われる熱剥離テープで被覆した後、この
負極Bを前記ゲル化成分含有電解液に減圧下で1分間浸
漬して、ゲル化成分含有電解液を含浸させた後、ポリエ
チレン製の袋に入れて密閉した。つぎに、そのポリエチ
レン製袋の外側から、上記負極Bの負極合剤層形成部分
が配置する側にフュージョンUVシステムズ・ジャパン
(株)製の紫外線照射装置を用いて、紫外線を1W/c
2 の照度で10秒間照射し、電解液中のモノマー成分
を重合させるとともに、電解液をゲル化してゲル状ポリ
マー電解質とした。このゲル状ポリマー電解質を保持さ
せた負極Bを袋から取り出し、そのリード部の負極端子
との接続に用いる部分に150℃の熱風を吹き付けるこ
とによって熱剥離テープを該部分から剥がし、ポリマー
電解質保持負極Bを得た。
Preparation of polymer electrolyte-holding negative electrode B: A polyimide tape having a thickness of 50 μm and a width of 3 mm was attached to both sides of the negative electrode B prepared as described above so as to extend over the negative electrode mixture layer forming portion and the lead portion. To prevent short circuits and maintain the strength of the terminals. Further, after covering all surfaces of a portion of the lead portion used for connection with the negative electrode terminal with a heat release tape which loses the adhesiveness of the adhesive surface due to heat, the negative electrode B was decompressed into the gelled component-containing electrolytic solution. After immersion for 1 minute in the lower part to impregnate the electrolytic solution containing the gelling component, the resultant was put in a polyethylene bag and sealed. Next, from the outside of the polyethylene bag, ultraviolet rays were irradiated at 1 W / c by using an ultraviolet irradiation device manufactured by Fusion UV Systems Japan Co., Ltd. on the side where the negative electrode mixture layer forming portion of the negative electrode B was arranged.
Irradiation was performed for 10 seconds at an illuminance of m 2 to polymerize the monomer components in the electrolyte and gel the electrolyte to form a gel polymer electrolyte. The negative electrode B holding the gelled polymer electrolyte is taken out of the bag, and a hot air of 150 ° C. is blown to a portion of the lead portion used for connection with the negative electrode terminal, thereby peeling off the thermal peeling tape from the portion, and the polymer electrolyte holding negative electrode. B was obtained.

【0029】つぎに、前記のようにして作製したポリマ
ー電解質保持正極5枚と、ポリマー電解質保持負極A4
枚と、ポリマー電解質保持負極B2枚を用意し、ポリマ
ー電解質保持負極B、ポリマー電解質保持正極、ポリマ
ー電解質保持負極A、ポリマー電解質保持正極、ポリマ
ー電解質保持負極A、ポリマー電解質保持正極、ポリマ
ー電解質保持負極A、ポリマー電解質保持正極、ポリマ
ー電解質保持負極A、ポリマー電解質保持正極、ポリマ
ー電解質保持負極Bの順に積層して電極積層体を得た。
この時、2枚のポリマー電解質保持負極Bの負極合剤層
形成部分は、いずれも電極積層体の内部側を向くように
して積層した。つまり、2枚のポリマー電解質保持負極
Bの厚さ10μmの銅箔からなる負極集電体を電極積層
体の外面側を向くように配置した。
Next, five polymer electrolyte-holding positive electrodes prepared as described above and a polymer electrolyte-holding negative electrode A4 were prepared.
Sheets and two polymer electrolyte-holding anodes B are prepared, and a polymer electrolyte-holding anode B, a polymer electrolyte-holding cathode, a polymer electrolyte-holding anode A, a polymer electrolyte-holding cathode, a polymer electrolyte-holding anode A, a polymer electrolyte-holding cathode, and a polymer electrolyte-holding anode A, a polymer electrolyte holding positive electrode, a polymer electrolyte holding negative electrode A, a polymer electrolyte holding positive electrode, and a polymer electrolyte holding negative electrode B were laminated in this order to obtain an electrode laminate.
At this time, the negative electrode mixture layer forming portions of the two polymer electrolyte-holding negative electrodes B were laminated such that both faced the inside of the electrode laminate. That is, the two negative electrode current collectors made of a copper foil having a thickness of 10 μm of the polymer electrolyte holding negative electrode B were arranged so as to face the outer surface of the electrode laminate.

【0030】この電極積層体では、ポリマー電解質保持
正極とポリマー電解質保持負極とを積層しているので、
正極に保持させたポリマー電解質と負極に保持させたポ
リマー電解質とが正極と負極との間にポリマー電解質
(特に正極の周囲に支持体として配置したポリブチレン
テレフタレート不織布の内部空孔や周囲にポリマー電解
質が高密度に存在する)が介在した状態で正極と負極と
が積層されている。
In this electrode laminate, since the polymer electrolyte holding positive electrode and the polymer electrolyte holding negative electrode are stacked,
The polymer electrolyte held on the positive electrode and the polymer electrolyte held on the negative electrode are placed between the positive electrode and the negative electrode. The polymer electrolyte (especially, the polymer electrolyte is placed inside and around the polybutylene terephthalate nonwoven fabric placed as a support around the positive electrode) Are present at a high density) and the positive electrode and the negative electrode are laminated.

【0031】この電極積層体を図4に基づいて説明する
が、この電極積層体を構成するために積層した電極は、
上記のようにポリマー電解質を保持させた正極とポリマ
ー電解質を保持させた負極であり、結果的に正極と負極
との間のポリマー電解質が介在している状態になるの
で、この図4では正極1と負極2との間にポリマー電解
質3を介在させた状態のものとして説明する。すなわ
ち、この図4に示す電極積層体は、一番下側に負極2
(この負極2は、負極B、つまり片面塗布負極に基づく
ものである)が配置し、その上に、ポリマー電解質3を
介して、正極1、負極2、正極1、負極2、正極1、負
極2、正極1、負極2、正極1、負極2(この負極2
は、負極B、つまり、片面塗布負極に基づくものであ
り、最外層の2枚の負極2以外は、すべて負極A、つま
り、両面塗布負極に基づくものである)の順に積層され
ている。なお、この図4では、上記の理由により、正極
1と負極2との間に白抜きでポリマー電解質3を示した
が、以後の図では、このポリマー電解質3の図示を省略
する。
This electrode laminate will be described with reference to FIG. 4. The electrodes laminated to form this electrode laminate are:
As described above, the positive electrode holding the polymer electrolyte and the negative electrode holding the polymer electrolyte result in a state in which the polymer electrolyte is interposed between the positive electrode and the negative electrode. The description will be made assuming that the polymer electrolyte 3 is interposed between the anode and the negative electrode 2. That is, the electrode laminate shown in FIG.
(This negative electrode 2 is based on a negative electrode B, that is, a single-sided coated negative electrode), and a positive electrode 1, a negative electrode 2, a positive electrode 1, a negative electrode 2, a positive electrode 1, a negative electrode 1, 2, positive electrode 1, negative electrode 2, positive electrode 1, negative electrode 2 (this negative electrode 2
Are based on the negative electrode B, that is, based on the single-sided coated negative electrode, and all the layers except the outermost two negative electrodes 2 are stacked on the negative electrode A, that is, based on the double-sided coated negative electrode). In FIG. 4, the polymer electrolyte 3 is shown in white between the positive electrode 1 and the negative electrode 2 for the above reason, but illustration of the polymer electrolyte 3 is omitted in the subsequent figures.

【0032】正極端子にはアルミニウムとニッケルとの
幅5mm、厚さ0.1mmのクラッド材を用い、この正
極端子の一方の端部と上記電極積層体の正極のリード部
の積層体とを、溶接時間75msec、圧力2kg/c
2 、アンプリチュード60%の条件下で超音波溶接し
た。また、負極端子には銅とニッケルとの幅5mm、厚
さ0.1mmのクラッド材を用い、この負極端子の一方
の端部と負極のリード部の積層体とを溶接時間120m
sec、圧力2kg/cm2 、アンプリチュード60%
の条件下で超音波溶接した。
For the positive electrode terminal, a clad material of aluminum and nickel having a width of 5 mm and a thickness of 0.1 mm was used, and one end of the positive electrode terminal and the laminate of the positive electrode lead portion of the electrode laminate were Welding time 75msec, pressure 2kg / c
Ultrasonic welding was performed under the conditions of m 2 and amplitude of 60%. For the negative electrode terminal, a clad material of copper and nickel having a width of 5 mm and a thickness of 0.1 mm was used, and one end of the negative electrode terminal and the laminate of the negative electrode lead portion were welded for 120 m.
sec, pressure 2kg / cm 2 , amplitude 60%
Ultrasonic welding under the following conditions.

【0033】上記電極積層体の封止に際して用いられる
外装材は、図5に示すように、保護フィルム4a、金属
箔4b、熱融着性樹脂フィルム4cの3層ラミネートフ
ィルムからなり、この実施例では、上記保護フィルム4
aとして厚さ30μmのナイロンフィルムが用いられて
おり、金属箔4bとしては厚さ50μmのアルミニウム
箔が用いられ、熱融着性樹脂フィルム4cとしては厚さ
30μmの変性ポリオレフィンフィルムが用いられてい
て、上記ナイロンフィルムはアルミニウム箔の損傷や腐
食を防ぎ、アルミニウム箔は水分やガスの透過を阻止
し、変性ポリオレフィンフィルムは接着層として作用す
る。この外装材4は上記電極積層体の封止にあたって2
枚用いられ、両者とも同じ構成のものであるが、そのう
ちの一方は上記電極積層体を収容しやすいようにあらか
じめ鍔付きの容器状に成形され、他方はプレート状をし
ていて、それぞれ変性ポリオレフィンフィルムを内面側
にして、電極積層体の周囲に配置することになるが、そ
のような電極積層体の周囲への配置に先立って、上記外
装材の正極のリード部と正極端子との接続部分およびそ
の近傍ならびに負極のリード部と正極端子との接続部分
およびその近傍に当たる部分に熱融着性樹脂フィルムを
貼り付けた。
As shown in FIG. 5, the exterior material used for sealing the electrode laminate is composed of a three-layer laminate film of a protective film 4a, a metal foil 4b, and a heat-fusible resin film 4c. Then, the protective film 4
A 30 μm-thick nylon film is used as a, a 50 μm-thick aluminum foil is used as the metal foil 4b, and a 30 μm-thick modified polyolefin film is used as the heat-fusible resin film 4c. The nylon film prevents the aluminum foil from being damaged or corroded, the aluminum foil prevents moisture or gas from permeating, and the modified polyolefin film acts as an adhesive layer. The exterior material 4 is used for sealing the electrode laminate 2.
Are used, and both have the same configuration, but one of them is formed in a container with a flange in advance so as to easily accommodate the electrode laminate, and the other is in the form of a plate. The film is disposed on the inner surface side and around the electrode laminate.Before such arrangement around the electrode laminate, a connection portion between the lead portion of the positive electrode and the positive terminal of the exterior material is provided. A heat-fusible resin film was attached to the vicinity thereof, the connection between the lead portion of the negative electrode and the positive electrode terminal, and the portion corresponding to the vicinity thereof.

【0034】すなわち、上記熱融着性樹脂フィルムとし
て、厚みが50μmで10mm×10mmの変性ポリオ
レフィンフィルムを上記2枚の外装材の熱融着性樹脂フ
ィルム側に貼り付けた。
That is, a modified polyolefin film having a thickness of 50 μm and a size of 10 mm × 10 mm was stuck to the heat-fusible resin film side of the two exterior materials as the heat-fusible resin film.

【0035】貼り付けた位置は、上記外装材の封止部で
正極端子が取り出される部分と負極端子が取り出される
部分の2箇所で、外装材の端部から電池内部側へ1mm
入ったところから正極のリード部と正極端子との接続部
の電池内部側の端部や負極のリード部と負極端子との接
続部の電池内部側の端部よりさらに3mm電池内部側に
入ったところまでである。
There are two locations where the positive terminal is taken out and the negative terminal is taken out at the sealing portion of the exterior material, and 1 mm from the end of the exterior material to the inside of the battery.
From the point of entry, the battery further enters the inside of the battery by 3 mm from the inside end of the battery at the connection between the positive electrode lead and the positive electrode terminal and the inside of the battery at the connection between the negative electrode lead and the negative electrode terminal. That's it.

【0036】そして、上記のように、その内面側の熱融
着性樹脂フィルムにさらに熱融着性樹脂フィルムとして
変性ポリオレフィンフィルムを貼り付けておいた外装材
を電極積層体の周囲に配置し、真空ポンプで電池内部を
減圧して、上記外装材などの接合部を加熱して外装材の
熱融着性樹脂フィルムとしての変性ポリオレフィンフィ
ルムおよびさらにそれを貼り付けた変性ポリオレフィン
フィルムを溶融させて熱融着して積層形ポリマー電解質
電池を作製した。
Then, as described above, an exterior material in which a modified polyolefin film is further adhered as a heat-fusible resin film to the heat-fusible resin film on the inner side thereof is arranged around the electrode laminate. The inside of the battery is depressurized by a vacuum pump, and the joint such as the above-mentioned exterior material is heated to melt the modified polyolefin film as the heat-fusible resin film of the exterior material and the modified polyolefin film to which the modified polyolefin film is adhered. By fusion, a laminated polymer electrolyte battery was produced.

【0037】図6は上記のように作製された積層形ポリ
マー電解質電池の平面図である。正極端子5と負極端子
6とは同じ方向に取り出されているが、両者の間に通常
15mmの間隔があって、通常の条件下では両者が接触
して短絡を引き起こすようなことはない。
FIG. 6 is a plan view of the laminated polymer electrolyte battery manufactured as described above. Although the positive electrode terminal 5 and the negative electrode terminal 6 are taken out in the same direction, there is usually a gap of 15 mm between them, and under normal conditions, they do not come into contact and cause a short circuit.

【0038】上記積層形ポリマー電解質電池の正極端子
取出部分の拡大断面図、すなわち、図6のX−X線断面
の拡大図を図7に示す。図7に示すように、正極1のリ
ード部1cと正極端子5との接続部およびその近傍と外
装材4との間には変性ポリオレフィンフィルムからなる
熱融着性樹脂フィルム7が介在し、その熱融着性樹脂フ
ィルム7の電池内部側の端部は正極端子5の電池内部側
の端部を越えてほぼ電極積層体の端部近くまで達してい
る。
FIG. 7 is an enlarged cross-sectional view of the portion of the stacked polymer electrolyte battery from which the positive electrode terminal is taken out, that is, an enlarged cross-sectional view taken along line XX of FIG. As shown in FIG. 7, a heat-fusible resin film 7 made of a modified polyolefin film is interposed between the connecting portion between the lead portion 1 c of the positive electrode 1 and the positive electrode terminal 5 and the vicinity thereof and the exterior material 4. The end of the heat-fusible resin film 7 on the inside of the battery extends almost beyond the end of the positive electrode terminal 5 on the inside of the battery to near the end of the electrode laminate.

【0039】また、上記積層形ポリマー電解質電池の負
極端子取出部分の拡大断面図、すなわち、図6のY−Y
線断面の拡大図を図8に示す。図8に示すように、負極
2のリード部2cと負極端子との接続部およびその近傍
と外装材4との間には変性ポリオレフィンフィルムから
なる熱融着性樹脂フィルム7が介在し、その熱融着性樹
脂フィルム7の電池内部側の端部は負極端子6の電池内
部側の端部を越えてほぼ電極積層体の端部近くにまで達
している。
FIG. 6 is an enlarged cross-sectional view of the portion where the negative electrode terminal is taken out of the laminated polymer electrolyte battery, that is, YY of FIG.
FIG. 8 shows an enlarged view of the line section. As shown in FIG. 8, a heat-fusible resin film 7 made of a modified polyolefin film is interposed between the connecting portion between the lead portion 2 c of the negative electrode 2 and the negative electrode terminal and the vicinity thereof and the package 4, The end of the fusible resin film 7 on the inside of the battery extends beyond the end of the negative electrode terminal 6 on the inside of the battery and almost reaches the end of the electrode laminate.

【0040】比較例1 正極のリード部と正極端子の端部との接続部およびその
近傍ならびに負極のリード部と負極端子との接続部およ
びその近傍に熱融着性樹脂フィルムを配設しなかった以
外は、実施例1と同様に積層形ポリマー電解質電池を作
製した。
COMPARATIVE EXAMPLE 1 A heat-fusible resin film was not provided at the connection between the lead portion of the positive electrode and the end of the positive electrode terminal and the vicinity thereof, and at the connection portion between the lead portion of the negative electrode and the negative electrode terminal and the vicinity thereof. A laminated polymer electrolyte battery was produced in the same manner as in Example 1 except for the above.

【0041】上記実施例1の電池と比較例1の電池をそ
れぞれ50個ずつ製造し、短絡が発生する電池個数を調
べた。その結果を表1に示す。ただし、表1への表示に
あたっては分母にそれぞれの電池において製造した全電
池個数を示し、分子に短絡が発生した電池個数を示す。
なお、短絡の発生は電池の抵抗を測定することによって
判断した。
The batteries of Example 1 and the battery of Comparative Example 1 were manufactured by 50 each, and the number of batteries in which a short circuit occurred was examined. Table 1 shows the results. However, in the display in Table 1, the denominator indicates the total number of batteries manufactured for each battery, and the numerator indicates the number of batteries having a short circuit.
The occurrence of the short circuit was determined by measuring the resistance of the battery.

【0042】[0042]

【表1】 [Table 1]

【0043】表1に示す結果から明らかなように、比較
例1では製造した50個の電池中の29個の電池に短絡
が発生したが、実施例1では短絡の発生がまったくなか
った。なお、前記図7や図8においては、外装材4の電
極積層体の本体部分が配置する部分から外装材4の封止
部分に至るまでの傾斜部分を変形させないで図示してい
るが、本発明では、減圧封止により上記傾斜部分がたと
え大きく変形したとしても、外装材4の内面側に貼り付
けた熱融着性樹脂フィルム7により正極1のリード部1
cと正極端子5との接続部の電池内部側の端部や負極2
のリード部2cと負極端子6との接続部の電池内部側の
端部が外装材4の熱融着性樹脂フィルムを突き破って短
絡を引き起こすのを防止することができる。
As is clear from the results shown in Table 1, short-circuit occurred in 29 of the 50 batteries manufactured in Comparative Example 1, but no short-circuit occurred in Example 1. In FIGS. 7 and 8, the inclined portion from the portion where the body portion of the electrode laminate of the exterior material 4 is arranged to the sealing portion of the exterior material 4 is shown without deformation. In the present invention, even if the inclined portion is greatly deformed by the decompression sealing, the lead portion 1 of the positive electrode 1 is formed by the heat-fusible resin film 7 adhered to the inner surface side of the exterior material 4.
c and the end of the connection between the positive electrode terminal 5 on the inside of the battery and the negative electrode 2
The end of the connection between the lead portion 2c and the negative electrode terminal 6 on the battery inside side can be prevented from breaking through the heat-fusible resin film of the exterior material 4 to cause a short circuit.

【0044】[0044]

【発明の効果】以上説明したように、本発明では、外装
材の減圧封止に伴う短絡の発生がない信頼性の高い積層
形ポリマー電解質電池を提供することができた。
As described above, according to the present invention, it is possible to provide a highly reliable laminated polymer electrolyte battery free from occurrence of a short circuit due to reduced-pressure sealing of an exterior material.

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

【図1】本発明の実施例1の積層形ポリマー電解質電池
を用いる正極を模式的に示す断面図である。
FIG. 1 is a cross-sectional view schematically showing a positive electrode using a laminated polymer electrolyte battery according to Example 1 of the present invention.

【図2】本発明の実施例1の積層形ポリマー電解質電池
に用いる負極Aを模式的に示す断面図である。
FIG. 2 is a cross-sectional view schematically showing a negative electrode A used in the laminated polymer electrolyte battery of Example 1 of the present invention.

【図3】本発明の実施例1の積層形ポリマー電解質電池
に用いる負極Bを模式的に示す断面図である。
FIG. 3 is a cross-sectional view schematically showing a negative electrode B used in the laminated polymer electrolyte battery of Example 1 of the present invention.

【図4】本発明の実施例1の積層形ポリマー電解質電池
に用いる電極積層体を模式的に示す断面図である。
FIG. 4 is a cross-sectional view schematically showing an electrode laminate used for the laminated polymer electrolyte battery of Example 1 of the present invention.

【図5】本発明の実施例1の積層形ポリマー電解質電池
に用いる外装材を模式的に示す断面図である。
FIG. 5 is a cross-sectional view schematically showing an exterior material used for the laminated polymer electrolyte battery of Example 1 of the present invention.

【図6】本発明の実施例1の積層形ポリマー電解質電池
を模式的に示す平面図である。
FIG. 6 is a plan view schematically showing a laminated polymer electrolyte battery of Example 1 of the present invention.

【図7】本発明の実施例1の積層形ポリマー電解質電池
の正極のリード部と正極端子との接続部分およびその近
傍を模式的に示す図であって、図6のX−X線断面の拡
大図である。
FIG. 7 is a diagram schematically showing a connection portion between the lead portion of the positive electrode and the positive electrode terminal of the laminated polymer electrolyte battery according to the first embodiment of the present invention and the vicinity thereof, taken along the line XX in FIG. 6; It is an enlarged view.

【図8】本発明の実施例1の積層形ポリマー電解質電池
の負極のリード部と負極端子との接続部分およびその近
傍を模式的に示す断面図であって、図6のY−Y線断面
の拡大図である。
8 is a cross-sectional view schematically showing a connection portion between a lead portion of a negative electrode and a negative electrode terminal of the laminated polymer electrolyte battery of Example 1 of the present invention and the vicinity thereof, and is a cross-sectional view taken along line YY of FIG. FIG.

【図9】従来法により電極積層体を外装材で封止すると
きの状態の要部を示す断面図である。
FIG. 9 is a cross-sectional view showing a main part in a state when the electrode laminate is sealed with a packaging material by a conventional method.

【図10】従来法により外装材で電極積層体を減圧封止
した状態を模式的に示す断面図である。
FIG. 10 is a cross-sectional view schematically showing a state in which an electrode laminate is sealed under reduced pressure with a packaging material by a conventional method.

【符号の説明】[Explanation of symbols]

1 正極 1a 正極集電体 1b 正極合剤層 1c リード部 2 負極 2a 負極集電体 2b 負極合剤層 2c リード部 3 ポリマー電解質 4 外装材 4a 保護フィルム 4b 金属箔 4c 熱融着性樹脂フィルム 5 正極端子 6 負極端子 7 熱融着性樹脂フィルム DESCRIPTION OF SYMBOLS 1 Positive electrode 1a Positive electrode collector 1b Positive electrode mixture layer 1c Lead part 2 Negative electrode 2a Negative electrode collector 2b Negative electrode mixture layer 2c Lead part 3 Polymer electrolyte 4 Outer material 4a Protective film 4b Metal foil 4c Heat-fusible resin film 5 Positive terminal 6 Negative terminal 7 Heat-fusible resin film

Claims (1)

【特許請求の範囲】[Claims] 【請求項1】 正極と負極とをそれらの間にポリマー電
解質を介在させて積層した電極積層体を、保護フィルム
と金属箔と熱融着性樹脂フィルムとのラミネートフィル
ムからなる外装材で封止する構造の積層形ポリマー電解
質電池において、正極のリード部と正極端子との接続部
およびその近傍ならびに負極のリード部と負極端子との
接続部およびその近傍に上記外装材を構成するラミネー
トフィルムの熱融着性樹脂フィルムと同一材質の熱融着
性樹脂フィルムを配設して外装材の減圧封止による変形
によって生じる短絡の発生を防止したことを特徴とする
積層形ポリマー電解質電池。
1. An electrode laminate in which a positive electrode and a negative electrode are laminated with a polymer electrolyte interposed therebetween is sealed with an exterior material composed of a laminate film of a protective film, a metal foil, and a heat-fusible resin film. In the laminated polymer electrolyte battery having the structure described above, the heat of the laminated film constituting the above-mentioned exterior material is formed in the vicinity of the connection between the lead portion of the positive electrode and the positive electrode terminal and the vicinity thereof and the connection portion between the lead portion of the negative electrode and the negative electrode terminal and the vicinity thereof. A laminated polymer electrolyte battery in which a heat-fusible resin film of the same material as the heat-fusible resin film is provided to prevent occurrence of a short circuit caused by deformation of the exterior material due to reduced-pressure sealing.
JP30622099A 1999-10-28 1999-10-28 Laminate polymer electrolyte battery Withdrawn JP2001126678A (en)

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KR20030032541A (en) * 2001-10-18 2003-04-26 삼성에스디아이 주식회사 Lithium secondary battery
EP1455400A2 (en) 2003-03-03 2004-09-08 NEC Lamilion Energy, Ltd. Film covered battery
JP2004319099A (en) * 2003-04-11 2004-11-11 Sii Micro Parts Ltd Electrochemical cell
JP2005116228A (en) * 2003-10-03 2005-04-28 Nec Lamilion Energy Ltd Heat-fusing method of laminate film, manufacturing method of film coating battery, and heat-fusing device for laminate film
WO2005091398A1 (en) * 2004-03-23 2005-09-29 Nec Lamilion Energy, Ltd. Film-packaged electric device and its manufacturing method
JP2005317315A (en) * 2004-04-28 2005-11-10 Pionics Co Ltd Positive electrode terminal for lithium secondary battery
US20060194103A1 (en) * 2003-08-08 2006-08-31 Makihiro Otohata Film-Covered Battery And Fabrication Method
CN100353592C (en) * 2003-11-06 2007-12-05 日本电气株式会社 Laminated battery
JP2008084666A (en) * 2006-09-27 2008-04-10 Hitachi Maxell Ltd Laminated nonaqueous secondary battery
US7910241B2 (en) * 2004-09-22 2011-03-22 Nissan Motor Co., Ltd. Battery outer case for receiving a flat battery pack joined by seam-rolling
JP2020057485A (en) * 2018-09-28 2020-04-09 積水化学工業株式会社 Laminate-type secondary battery and method for producing the same
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KR20030032541A (en) * 2001-10-18 2003-04-26 삼성에스디아이 주식회사 Lithium secondary battery
EP1455400A2 (en) 2003-03-03 2004-09-08 NEC Lamilion Energy, Ltd. Film covered battery
US7498099B2 (en) 2003-03-03 2009-03-03 Nec Corporation Film covered battery
JP2004319099A (en) * 2003-04-11 2004-11-11 Sii Micro Parts Ltd Electrochemical cell
US20060194103A1 (en) * 2003-08-08 2006-08-31 Makihiro Otohata Film-Covered Battery And Fabrication Method
JP4775555B2 (en) * 2003-08-08 2011-09-21 日本電気株式会社 Film-clad battery and manufacturing method thereof
US7931982B2 (en) 2003-08-08 2011-04-26 Nec Corporation Battery with laminated film covering and fabrication method
JP4666131B2 (en) * 2003-10-03 2011-04-06 日本電気株式会社 LAMINATE FILM HEAT FUSION METHOD, FILM PACKAGE BATTERY MANUFACTURING METHOD, AND LAMINATE FILM HEAT FUSION DEVICE
JP2005116228A (en) * 2003-10-03 2005-04-28 Nec Lamilion Energy Ltd Heat-fusing method of laminate film, manufacturing method of film coating battery, and heat-fusing device for laminate film
CN100353592C (en) * 2003-11-06 2007-12-05 日本电气株式会社 Laminated battery
WO2005091398A1 (en) * 2004-03-23 2005-09-29 Nec Lamilion Energy, Ltd. Film-packaged electric device and its manufacturing method
US7736801B2 (en) 2004-03-23 2010-06-15 Nec Corporation Film covered electric device and method of manufacturing the same
JP2005317315A (en) * 2004-04-28 2005-11-10 Pionics Co Ltd Positive electrode terminal for lithium secondary battery
US7910241B2 (en) * 2004-09-22 2011-03-22 Nissan Motor Co., Ltd. Battery outer case for receiving a flat battery pack joined by seam-rolling
US8747490B2 (en) 2004-09-22 2014-06-10 Nissan Motor Co., Ltd. Assembling method for battery outer case for receiving a flat battery pack joined by seam-rolling
JP2008084666A (en) * 2006-09-27 2008-04-10 Hitachi Maxell Ltd Laminated nonaqueous secondary battery
JP2020057485A (en) * 2018-09-28 2020-04-09 積水化学工業株式会社 Laminate-type secondary battery and method for producing the same
KR20220135569A (en) * 2021-03-30 2022-10-07 주식회사 엘지에너지솔루션 Pouch type secondary battery and battery module having the same
EP4068445A3 (en) * 2021-03-30 2023-05-24 LG Energy Solution, Ltd. Pouch-type secondary battery and battery module
KR102566013B1 (en) * 2021-03-30 2023-08-10 주식회사 엘지에너지솔루션 Pouch type secondary battery and battery module having the same
WO2022270761A1 (en) * 2021-06-24 2022-12-29 주식회사 엘지에너지솔루션 Electrode tab protective tape and secondary battery comprising same

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