JP3496090B2 - Exterior material for secondary battery and method of manufacturing the same - Google Patents
Exterior material for secondary battery and method of manufacturing the sameInfo
- Publication number
- JP3496090B2 JP3496090B2 JP16748399A JP16748399A JP3496090B2 JP 3496090 B2 JP3496090 B2 JP 3496090B2 JP 16748399 A JP16748399 A JP 16748399A JP 16748399 A JP16748399 A JP 16748399A JP 3496090 B2 JP3496090 B2 JP 3496090B2
- Authority
- JP
- Japan
- Prior art keywords
- film
- acid
- modified polyolefin
- metal foil
- secondary 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.)
- Expired - Fee Related
Links
Classifications
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Landscapes
- Sealing Battery Cases Or Jackets (AREA)
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、リチウムイオン二
次電池の外装材として好適に使用しうる外装材料料及び
その製造方法に関し、特にポリマー電解質や電解質溶液
等の各種電解質が封入されてなる、シート状で薄型のリ
チウムイオン二次電池の外装材として、好適に使用しう
る外装材料の製造方法に関するものである。なお、本発
明においては、二次電池に適用しうるように所定の寸法
に裁断されたものを「外装材」と表現し、所定の寸法に
裁断される前のものを「外装材料」と表現している。従
って、外装材と外装材料とは、寸法の相違だけで、実質
的には同一のものである。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a packaging material that can be preferably used as a packaging material for a lithium ion secondary battery and a method for producing the same, and in particular, various electrolytes such as polymer electrolytes and electrolyte solutions are encapsulated. The present invention relates to a method for manufacturing an exterior material that can be suitably used as an exterior material for a sheet-shaped thin lithium-ion secondary battery. In the present invention, what is cut into a predetermined size so as to be applicable to a secondary battery is referred to as an "exterior material", and one that is not cut into a predetermined size is referred to as an "exterior material". is doing. Therefore, the exterior material and the exterior material are substantially the same except for the size.
【０００２】[0002]
【従来の技術】シート状で薄型のポリマーリチウムイオ
ン二次電池等の二次電池は、近年、移動体通信機器，ノ
ートブック型パソコン，ヘッドフォンステレオ，カムコ
ーダー等のエレクトロニクス機器の小型軽量化に伴い、
その駆動源として重宝されている。この二次電池は、例
えば、図１に示したような構成となっている。即ち、正
極集電体２，正極３，隔離材（セパレーター）４，負極
５，負極集電体６の順で積層された積層体を、外装材
１，１で包装収納した構成となっている。そして、外装
材１，１は、端部７，７において熱封緘されている。2. Description of the Related Art Secondary batteries such as thin sheet-like polymer lithium-ion secondary batteries have been used in recent years as electronic devices such as mobile communication devices, notebook computers, headphone stereos, and camcorders have become smaller and lighter.
It is useful as a drive source. This secondary battery has, for example, a configuration shown in FIG. That is, the positive electrode current collector 2, the positive electrode 3, the separator (separator) 4, the negative electrode 5, and the negative electrode current collector 6 are laminated in this order and packaged and housed in the exterior materials 1 and 1. . The exterior materials 1 and 1 are heat-sealed at the end portions 7 and 7.
【０００３】外装材１は、一般的に、図２に示すよう
に、外装材本体８と熱封緘層９とが積層貼着された態様
となっている。外装材本体８としては、金属箔，金属蒸
着フィルム，耐熱性フィルム等が用いられている。ま
た、熱封緘層９としては、酸変成ポリオレフィンフィル
ムが用いられている。外装材本体８と熱封緘層９とは、
直接、貼着される場合もあるし、ポリウレタン系接着剤
等の接着剤層（図示せず）を介して、貼着される場合も
ある。As shown in FIG. 2, the exterior material 1 generally has a form in which an exterior material body 8 and a heat sealing layer 9 are laminated and adhered. As the exterior material body 8, a metal foil, a metal vapor deposition film, a heat resistant film, or the like is used. An acid-modified polyolefin film is used as the heat-sealing layer 9. The exterior material body 8 and the heat sealing layer 9 are
It may be directly attached, or may be attached via an adhesive layer (not shown) such as a polyurethane adhesive.
【０００４】このような外装材１は、二次電池の端部７
で、熱封緘層９を溶融させて熱封緘される。しかし、し
ばしば、熱封緘層９と外装材本体８とが剥離（デラミと
も言う）を起こし、液漏れを起こすということがあっ
た。このような液漏れは、二次電池が組み込まれたエレ
クトロニクス機器に、致命的な障害を与えるものであ
る。Such an exterior material 1 is used as an end portion 7 of a secondary battery.
Then, the heat-sealing layer 9 is melted and heat-sealed. However, the heat-sealing layer 9 and the exterior material body 8 often peeled off (also referred to as delamination) to cause liquid leakage. Such liquid leakage gives a fatal obstacle to the electronic device in which the secondary battery is incorporated.
【０００５】[0005]
【発明が解決しようとする課題】本発明者は、熱封緘層
９と外装材本体８とが、何故に剥離するのか検討した。
その結果、二次電池に収納されている積層体は、イオン
性塩を含む電解質が含浸された状態となっており，この
イオン性塩が、熱封緘層２を透過し、外装材本体８を腐
食するためであることが判明した。即ち、イオン性塩と
して、特に伝導度の大きいＬｉＰＦ6を用いると、若干
の水分と反応してフッ酸（オキシフッ化リン化合物等を
含む酸性物質）を生成し、これが熱封緘層２を透過し、
外装材本体８と熱封緘層２との密着を破壊し、剥離を生
じることが判明した。また、熱封緘層９と外装材本体８
との間に、接着剤層が介在していても、フッ酸は接着剤
層をも透過し、前記と同様の原理によって剥離が生じる
ことも判明した。The present inventor examined why the heat sealing layer 9 and the exterior body 8 are separated from each other.
As a result, the laminated body housed in the secondary battery is in a state of being impregnated with an electrolyte containing an ionic salt, and the ionic salt penetrates the heat sealing layer 2 to cause the exterior material body 8 to pass through. It turned out to be due to corrosion. That is, when LiPF 6 having a particularly high conductivity is used as the ionic salt, it reacts with a little water to generate hydrofluoric acid (an acidic substance containing a phosphorus oxyfluoride compound etc.), which permeates the heat sealing layer 2. ,
It was found that the adhesion between the exterior material body 8 and the heat-sealing layer 2 was destroyed and peeling occurred. In addition, the heat sealing layer 9 and the exterior body 8
It was also found that the hydrofluoric acid penetrates through the adhesive layer even if the adhesive layer is interposed between and, and peeling occurs according to the same principle as described above.
【０００６】そこで、本発明者等は、外装材本体８の表
面に、耐蝕性皮膜を設ければ、このような剥離を防止し
うるのではないかと考えた。具体的には、外装材本体８
としては、金属箔が用いられることが多いため、金属箔
本体表面に耐蝕性皮膜として、アルマイト処理皮膜，ジ
ルコニウム化成処理皮膜，チタン化成処理皮膜又はクロ
ム化成処理皮膜を設け、これを外装材本体８（金属箔）
として実験を行った。その結果、予期せぬことに、クロ
ム化成処理皮膜のみが、上記した剥離を有効に防止しう
ることが判明した。即ち、クロム化成処理皮膜と同様の
耐蝕性を持つと考えられているアルマイト処理皮膜，ジ
ルコニウム化成処理皮膜及びチタン化成処理皮膜は、上
記した剥離を有効に防止できず、二次電池の外装材とし
て適しておらず、クロム化成処理皮膜のみが二次電池の
外装材に適していることが判明したのである。本発明
は、このような予期せぬ発見に基づいてなされたもので
ある。Therefore, the present inventors have thought that such peeling can be prevented by providing a corrosion-resistant film on the surface of the outer casing body 8. Specifically, the exterior material body 8
Since a metal foil is often used, an alumite treatment film, a zirconium chemical conversion treatment film, a titanium chemical conversion treatment film or a chrome chemical conversion treatment film is provided on the surface of the metal foil main body as a corrosion resistant coating, and this is used as the exterior material main body 8 (Metal foil)
The experiment was conducted as. As a result, it has been unexpectedly found that only the chromium chemical conversion coating can effectively prevent the above-mentioned peeling. That is, the alumite treatment film, zirconium conversion treatment film, and titanium conversion treatment film, which are considered to have the same corrosion resistance as the chromium conversion treatment film, cannot effectively prevent the above-mentioned peeling, and are used as an exterior material for secondary batteries. It was not suitable, and it was found that only the chromium chemical conversion coating was suitable as the exterior material for the secondary battery. The present invention has been made based on such an unexpected discovery.
【０００７】[0007]
【課題を解決するための手段】即ち、本発明は、金属箔
本体と、該金属箔本体の少なくとも片面全面にクロメー
ト処理により形成されたクロム化成処理皮膜とからなる
金属箔の、該クロム化成処理皮膜側全面に酸変成ポリオ
レフィンフィルムよりなる熱封緘層が設けられているこ
とを特徴とする二次電池用外装材料に関するものであ
る。That is, the present invention provides a chrome chemical conversion treatment of a metal foil comprising a metal foil main body and a chrome chemical conversion treatment film formed by chromate treatment on at least one entire surface of the metal foil main body. The present invention relates to an exterior material for a secondary battery, which is characterized in that a heat-sealing layer made of an acid-modified polyolefin film is provided on the entire surface on the film side.
【０００８】本発明においては、外装材本体８として金
属箔１０を用いる。そして、金属箔１０としては、金属
箔本体１１の少なくとも片面全面に、クロメート処理に
より形成されたクロム化成処理皮膜１２が設けられてな
るものを用いる。金属箔本体１１としては、一般的に
は、安価で軽量なアルミニウム箔が用いられるが、その
他に、ステンレス箔，鉄箔或いは銅箔であっても差し支
えない。金属箔本体１１には、金属箔本体表面が酸化さ
れることによって生成した酸化皮膜（自然酸化皮膜）が
設けられていても良いし、アルマイト処理によって生成
した酸化皮膜（陽極酸化皮膜）が設けられていても良
い。このような酸化皮膜が設けられていると、絶縁層と
なり、二次電池が短絡するのを積極的に防止しうるの
で、好ましいことである。In the present invention, the metal foil 10 is used as the exterior material body 8. As the metal foil 10, a metal foil body 11 having a chromium chemical conversion coating 12 formed by a chromate treatment on at least one entire surface thereof is used. In general, inexpensive and lightweight aluminum foil is used as the metal foil body 11, but stainless foil, iron foil, or copper foil may be used instead. The metal foil body 11 may be provided with an oxide film (natural oxide film) formed by oxidizing the surface of the metal foil body, or may be provided with an oxide film (anodized film) formed by alumite treatment. It may be. It is preferable that such an oxide film is provided because it serves as an insulating layer and can positively prevent a short circuit in the secondary battery.
【０００９】金属箔本体１１の片面又は両面には、クロ
ム化成処理皮膜１２が設けられている。クロム化成処理
皮膜は、従来公知のクロメート処理によって形成される
ものである。そして、クロム化成処理皮膜中のクロム含
有量が、クロム換算で５〜５０ｍｇ／ｍ2程度にすれば
良い。具体的なクロメート処理の方法としては、酸化ク
ロムとポリアクリル酸とを主成分とする水溶液を、金属
箔本体１１の表面に塗布し、加熱及び乾燥する方法が好
ましい。その他にも、従来公知のクロメート処理、例え
ば、酸化クロムを主成分とする水溶液や、酸化クロムと
リン酸とを主成分とする水溶液等を塗布して、クロメー
ト処理を行っても良い。A chromium chemical conversion coating 12 is provided on one or both sides of the metal foil body 11. The chromium chemical conversion coating is formed by a conventionally known chromate treatment. Then, the chromium content in the chromium conversion coating may be about 5 to 50 mg / m 2 in terms of chromium. As a specific chromate treatment method, a method of applying an aqueous solution containing chromium oxide and polyacrylic acid as main components to the surface of the metal foil body 11, and heating and drying is preferable. In addition, a conventionally known chromate treatment, for example, an aqueous solution containing chromium oxide as a main component, an aqueous solution containing chromium oxide and phosphoric acid as a main component, or the like may be applied to perform the chromate treatment.
【００１０】そして、クロム化成処理皮膜１２側全面に
は、酸変成ポリオレフィンフィルムよりなる熱封緘層９
が設けられている。ここで、酸変成ポリオレフィンと
は、ポリエチレン又はポリプロピレンの側鎖にジカルボ
ン酸を付加したものであり、一般的にはポリプロピレン
の側鎖にマレイン酸又は無水マレイン酸を付加させたも
のである。本発明では、特に無水マレイン酸を付加させ
たものが好ましく、従って、無水マレイン酸変成ポリオ
レフィンフィルムを用いるのが好ましい。The heat-sealing layer 9 made of an acid-modified polyolefin film is formed on the entire surface of the chromium conversion coating 12 side.
Is provided. Here, the acid-modified polyolefin is a polyethylene or polypropylene having a side chain added with a dicarboxylic acid, and is generally a polypropylene having a side chain added with maleic acid or maleic anhydride. In the present invention, those to which maleic anhydride is added are particularly preferable, and therefore it is preferable to use a maleic anhydride modified polyolefin film.
【００１１】クロム化成処理皮膜１２と熱封緘層９と
は、図３に示す如く、直接貼着されていても良い。ま
た、任意の接着剤を用いて貼着されていても良い。任意
の接着材を用いる場合、種々の方法を採用しうるが、特
に以下に示すような特別に工夫された方法を採用するの
が好ましい。この特別に工夫された貼着方法は、本件出
願人が既に提案した特許第２５６７３６０号に係る発明
を利用した方法である。即ち、まず、クロム化成処理皮
膜１２表面全面に、酸変成ポリオレフィンを固形分とす
るオルガノゾルを塗布する。このオルガノゾルは、有機
液体中に酸変成ポリオレフィンがコロイド状で分散して
いるコロイド溶液である。有機液体としては、炭化水素
系の液体が用いられ、主としてトルエンが用いられる。
また、オルガノゾルの固形分濃度は５〜５０重量％程度
である。The chromium conversion coating 12 and the heat sealing layer 9 may be directly adhered as shown in FIG. Further, it may be attached using an arbitrary adhesive. When an arbitrary adhesive is used, various methods can be adopted, but it is preferable to use a specially devised method as shown below. This specially devised sticking method is a method utilizing the invention of Japanese Patent No. 2567360 already proposed by the present applicant. That is, first, an organosol having a solid content of acid-modified polyolefin is applied to the entire surface of the chromium conversion coating 12. This organosol is a colloidal solution in which an acid-modified polyolefin is colloidally dispersed in an organic liquid. As the organic liquid, a hydrocarbon liquid is used, and mainly toluene is used.
The solid concentration of the organosol is about 5 to 50% by weight.
【００１２】このオルガノゾルが塗布された後、乾燥工
程に導入し、オルガノゾルを乾燥する。乾燥条件は、温
度１５０〜２２０℃、時間５〜４０秒程度である。この
乾燥工程により、オルガノゾルは固化し接着性皮膜１３
となる。オルガノゾルは酸変成ポリオレフィンがコロイ
ド状となって分散しているので、クロム化成処理皮膜１
２表面上に比較的均一に塗布され、均一な接着性皮膜１
３が得られる。この後、接着性皮膜１３表面上に単層の
酸変成ポリオレフィンフィルムを重合し、圧着すること
によって、クロム化成処理皮膜１２（即ち、金属箔１
０）と酸変成ポリオレフィンフィルムとが貼着される。
接着性皮膜１３表面上に酸変成ポリオレフィンフィルム
１４を圧着する条件としては、１６０〜２４０℃の加熱
下で、圧力０．５〜２ｋｇ／ｃｍ2、時間０．５〜３秒
程度が良い。この酸変成ポリオレフィンフィルムは、オ
ルガノゾル中の酸変成ポリオレフィンと同種のもので形
成されているものである。そして、この貼着された酸変
成ポリオレフィンフィルムが熱封緘層となる。なお、オ
ルガノゾル中の酸変成ポリオレフィン及び酸変成ポリオ
レフィンフィルムは、いずれも無水マレイン酸変成ポリ
プロピレンよりなるものを採用するのが好ましい。After this organosol is applied, it is introduced into a drying step to dry the organosol. The drying conditions are a temperature of 150 to 220 ° C. and a time of about 5 to 40 seconds. By this drying step, the organosol is solidified and the adhesive film 13 is formed.
Becomes Since the acid-modified polyolefin is colloidal and dispersed in the organosol, the chromium chemical conversion coating 1
2 Adhesive film that is applied uniformly on the surface and has a uniform adhesion.
3 is obtained. After that, a single-layer acid-modified polyolefin film is polymerized on the surface of the adhesive film 13 and pressure-bonded to the chrome chemical conversion film 12 (that is, the metal foil 1).
0) and the acid-modified polyolefin film are attached.
As conditions for pressure-bonding the acid-modified polyolefin film 14 on the surface of the adhesive film 13, it is preferable that the pressure is 0.5 to 2 kg / cm 2 and the time is 0.5 to 3 seconds under heating at 160 to 240 ° C. This acid-modified polyolefin film is formed of the same kind as the acid-modified polyolefin in the organosol. Then, the attached acid-modified polyolefin film becomes a heat sealing layer. The acid-modified polyolefin and the acid-modified polyolefin film in the organosol are preferably both made of maleic anhydride-modified polypropylene.
【００１３】また、酸変成ポリオレフィンフィルムに代
えて、両面に酸変成ポリオレフィンフィルム９，９’が
貼合された三層ポリオレフィン系フィルム１４を用いて
も良い。この場合、接着性皮膜１３表面上にポリオレフ
ィン系フィルム１４が重合され、圧着することによって
クロム化成処理皮膜１２（即ち、金属箔１０）とポリオ
レフィン系フィルム１４とが貼着される。ポリオレフィ
ン系フィルム１４は、両面に、オルガノゾル中の酸変成
ポリオレフィンと同種の酸変成ポリオレフィンフィルム
を備えたものである。具体的には、ポリプロピレンフィ
ルム１５の両面に酸変成ポリオレフィンフィルム９，
９’を備えた、三層構造のポリオレフィン系フィルム１
４を用いるのが好ましい。また、ポリプロピレンフィル
ム１５に代えて、ポリエチレンフィルムやエチレン−酢
酸ビニル共重合体フィルム等を用いることができる。Further, instead of the acid-modified polyolefin film, a three-layer polyolefin film 14 having the acid-modified polyolefin films 9 and 9'bonded on both sides may be used. In this case, the polyolefin film 14 is polymerized on the surface of the adhesive film 13, and the chromium chemical conversion film 12 (that is, the metal foil 10) and the polyolefin film 14 are attached by pressure bonding. The polyolefin-based film 14 is provided with an acid-modified polyolefin film of the same type as the acid-modified polyolefin in the organosol on both sides. Specifically, the acid-modified polyolefin film 9 is formed on both sides of the polypropylene film 15,
Three-layer structure polyolefin-based film 1 having 9 '
It is preferable to use 4. Further, instead of the polypropylene film 15, a polyethylene film, an ethylene-vinyl acetate copolymer film or the like can be used.
【００１４】接着性皮膜１３表面上にポリオレフィン系
フィルム１４を圧着する条件も、１６０〜２４０℃の加
熱下で、圧力０．５〜２ｋｇ／ｃｍ2、時間０．５〜３
秒程度が良い。以上のようにして圧着すると、ポリオレ
フィン系フィルムの一方の面に存在する酸変成ポリオレ
フィンフィルム９’と、接着性皮膜１３とが貼着され
る。そして、ポリオレフィン系フィルムの他方の面に存
在する酸変成ポリオレフィンフィルム９が、熱封緘層と
なるのである。このようにして得られた二次電池用外装
材料の横断面図は、図４に示す如き態様になる。なお、
オルガノゾル中の酸変成ポリオレフィン及びポリオレフ
ィン系フィルム中の酸変成ポリオレフィンフィルムは、
いずれも無水マレイン酸変成ポリプロピレンよりなるも
のを採用するのが好ましい。The conditions under which the polyolefin film 14 is pressure-bonded onto the surface of the adhesive film 13 are also under heating at 160 to 240 ° C., pressure of 0.5 to 2 kg / cm 2 , and time of 0.5 to 3
Seconds are good. When pressure-bonded as described above, the acid-modified polyolefin film 9 ′ existing on one surface of the polyolefin film and the adhesive film 13 are attached. Then, the acid-modified polyolefin film 9 present on the other surface of the polyolefin film becomes the heat sealing layer. The cross-sectional view of the exterior material for a secondary battery obtained in this way has an aspect as shown in FIG. In addition,
The acid-modified polyolefin in the organosol and the acid-modified polyolefin film in the polyolefin-based film are
In each case, it is preferable to adopt a maleic anhydride modified polypropylene.
【００１５】クロム化成処理皮膜１２と熱封緘層９とが
直接貼着されている場合と、上記した特許第２５６７３
６０号に係る発明を利用した方法の場合とでは、後者の
方が、クロム化成処理皮膜１２と熱封緘層９とが強固に
貼着されるため、好ましいものである。即ち、後者の場
合、クロム化成処理皮膜１２と熱封緘層９とが直接貼着
の場合に比べて、オルガノゾルのクロム化成処理皮膜１
２に対する均一塗布性、オルガノゾル由来の接着性皮膜
１３と酸変成ポリオレフィンフィルムとの接着性が、い
ずれも良好なため、クロム化成処理皮膜１２と熱封緘層
９とが強固に貼着されるのである。The case where the chromium chemical conversion coating 12 and the heat sealing layer 9 are directly adhered to each other, and the case where the above-mentioned Japanese Patent No. 25673 is used.
In the case of the method utilizing the invention of No. 60, the latter is preferable because the chromium chemical conversion coating 12 and the heat sealing layer 9 are firmly adhered to each other. That is, in the latter case, compared with the case where the chromium chemical conversion coating 12 and the heat sealing layer 9 are directly attached, the organosol chromium chemical conversion coating 1
The uniform coating property with respect to 2 and the adhesive property between the organosol-derived adhesive film 13 and the acid-modified polyolefin film are both good, so that the chrome conversion treatment film 12 and the heat-sealing layer 9 are firmly adhered. .
【００１６】以上のようにして、少なくとも片面全面に
クロメート処理により形成されたクロム化成処理皮膜１
２を備えた金属箔１０と、この金属箔１０のクロム化成
処理皮膜１２側全面に設けられた酸変成ポリオレフィン
フィルム９とよりなる二次電池用外装材料が得られるの
である。特に、本件出願人が既に提案した特許第２５６
７３６０号に係る発明を利用すれば、少なくとも片面全
面にクロメート処理により形成されたクロム化成処理皮
膜１２を備えた金属箔１０と、この金属箔１０のクロム
化成処理皮膜１２側全面に設けられた酸変成ポリオレフ
ィンフィルム９とが、接着性皮膜１３（場合により、ポ
リオレフィン系フィルム１４の他の層を介在して）で強
固に貼着された二次電池用外装材料が得られるのであ
る。As described above, the chromium conversion coating 1 formed by chromate treatment on at least one entire surface
Thus, an outer packaging material for a secondary battery can be obtained, which is composed of the metal foil 10 provided with No. 2 and the acid-modified polyolefin film 9 provided on the entire surface of the metal foil 10 on the chromium chemical conversion coating 12 side. In particular, Patent No. 256 already proposed by the applicant
By using the invention according to JP 7360, at least one side total
A metal foil 10 having a chromium chemical conversion coating 12 formed on its surface by a chromate treatment, and an acid-modified polyolefin film 9 provided on the entire surface of the metal foil 10 on the chromium chemical conversion coating 12 side have an adhesive coating 13 ( In some cases, an outer packaging material for a secondary battery, which is firmly adhered with (through interposing other layers of the polyolefin-based film 14), is obtained.
【００１７】この二次電池用外装材料を用いて、二次電
池を得る方法の一例としては、以下のような方法が挙げ
られる。即ち、二次電池用外装材料を所望の大きさに裁
断した外装材２枚を用いて、熱封緘層である酸変成ポリ
オレフィン系フィルム９同士が当接するようにして積層
する。そして、一部を残し、他の端部７を熱封緘（即
ち、酸変成ポリオレフィン系フィルムの溶融圧着による
接着）して、袋を得る。そして、この袋の口から、正極
集電体２，正極３，隔離材４，負極５，負極集電体６の
順で積層された積層体を電解質で含浸し活性化させた二
次電池本体部分を収納する。最後に、二次電池本体部分
から延びているリード線を外部に出すようにして、袋の
口を再度、熱封緘すれば、二次電池が得られるのであ
る。なお、二次電池用外装材料の金属箔１０の他面、即
ち、熱封緘層９の不存在面に文字や模様等を印刷した
り、合成樹脂製のオーバーコート層をポリウレタン系接
着剤等で貼合しても良いことは、言うまでもない。As an example of a method for obtaining a secondary battery using this secondary battery exterior material, the following method can be mentioned. That is, two outer packaging materials obtained by cutting the outer packaging material for a secondary battery into a desired size are laminated so that the acid-modified polyolefin-based films 9 that are heat sealing layers are in contact with each other. Then, leaving a part, the other end 7 is heat-sealed (that is, the acid-modified polyolefin-based film is bonded by fusion bonding) to obtain a bag. Then, from the mouth of this bag, the secondary battery main body in which the positive electrode current collector 2, the positive electrode 3, the separator 4, the negative electrode 5, and the negative electrode current collector 6 are laminated in this order and impregnated with an electrolyte to be activated. Store the part. Finally, a secondary battery can be obtained by resealing the mouth of the bag with the lead wire extending from the main body of the secondary battery exposed to the outside. It should be noted that characters or patterns are printed on the other surface of the metal foil 10 of the exterior material for the secondary battery, that is, the non-existing surface of the heat sealing layer 9, or the synthetic resin overcoat layer is formed by a polyurethane adhesive or the like. It goes without saying that they can be pasted together.
【００１８】[0018]
【実施例】実施例１
金属箔本体として、厚さ３０μｍのアルミニウム箔を準
備した。一方、クロメート処理液として、酸化クロムと
ポリアクリル酸を主成分とする水溶液（クロム含有量は
６ｍｇ／ｃｃ）を準備した。そして、アルミニウム箔の
両面に、クロメート処理液を均一に塗布し、１５０℃で
１５秒間の条件で乾燥した。この結果、アルミニウム箔
表面に、クロム含有量が３０ｍｇ／ｍ2のクロム化成処
理皮膜が形成された金属箔を得た。次に、平均粒径６〜
８μｍの無水マレイン酸変成ポリプロピレン１５重量部
とトルエン８５重量部よりなるオルガノゾルを準備し
た。そして、これを金属箔の片面に（即ち、アルミニウ
ム箔両面に形成されたクロム化成処理皮膜の一方の表面
に）塗布し、２００℃で２０秒間の条件で乾燥し、厚さ
２μｍの接着性皮膜を得た。最後に、ポリオレフィン系
フィルムとして、厚さ３０μｍのポリプロピレンフィル
ムの両面に、厚さ１０μｍの無水マレイン酸変成ポリプ
ロピレンフィルムが貼合された、３層共押出フィルムを
準備した。そして、これを、温度２００℃、圧力２ｋｇ
／ｃｍ2、時間１秒間の圧着条件で、接着性皮膜表面に
圧着した。以上のようにして、クロム化成処理皮膜／ア
ルミニウム箔／クロム化成処理皮膜／接着性皮膜／無水
マレイン酸変成ポリプロピレンフィルム／ポリプロピレ
ンフィルム／無水マレイン酸変成ポリプロピレンフィル
ム（熱封緘層）の順で積層貼着された二次電池用外装材
料を得た。Example 1 An aluminum foil having a thickness of 30 μm was prepared as a metal foil body. On the other hand, as a chromate treatment liquid, an aqueous solution containing chromium oxide and polyacrylic acid as main components (chromium content: 6 mg / cc) was prepared. Then, the chromate treatment liquid was uniformly applied to both surfaces of the aluminum foil, and dried at 150 ° C. for 15 seconds. As a result, a metal foil having a chromium chemical conversion coating with a chromium content of 30 mg / m 2 formed on the surface of the aluminum foil was obtained. Next, the average particle size 6 to
An organosol comprising 15 parts by weight of 8 μm maleic anhydride modified polypropylene and 85 parts by weight of toluene was prepared. Then, this is applied to one surface of the metal foil (that is, one surface of the chrome chemical conversion coating formed on both surfaces of the aluminum foil), dried at 200 ° C. for 20 seconds, and an adhesive coating having a thickness of 2 μm. Got Finally, as a polyolefin-based film, a three-layer coextrusion film was prepared in which a maleic anhydride modified polypropylene film having a thickness of 10 μm was laminated on both sides of a polypropylene film having a thickness of 30 μm. And, this, temperature 200 ℃, pressure 2kg
The pressure-sensitive adhesive layer was pressure-bonded to the surface of the adhesive film under a pressure-bonding condition of / cm 2 for 1 second. As described above, chrome conversion treatment film / aluminum foil / chromium conversion treatment film / adhesive film / maleic anhydride modified polypropylene film / polypropylene film / maleic anhydride modified polypropylene film (heat sealing layer) are laminated in this order. The obtained exterior material for secondary battery was obtained.
【００１９】実施例２
３層共押出フィルムに代えて、厚さ５０μｍの無水マレ
イン酸変成ポリプロピレンフィルム単層を使用した他
は、実施例１と同様の方法で二次電池用外装材料を得
た。この場合は、無水マレイン酸変成ポリプロピレンフ
ィルム単層が熱封緘層となる。Example 2 An exterior material for a secondary battery was obtained in the same manner as in Example 1 except that a single layer of maleic anhydride modified polypropylene film having a thickness of 50 μm was used instead of the three-layer coextruded film. . In this case, the maleic anhydride-modified polypropylene film single layer serves as the heat sealing layer.
【００２０】比較例１
クロム化成処理皮膜を形成しない他は、実施例１と同様
の方法で二次電池用外装材料を得た。Comparative Example 1 An exterior material for a secondary battery was obtained in the same manner as in Example 1 except that the chromium conversion coating was not formed.
【００２１】比較例２
クロム化成処理皮膜を形成しない他は、実施例２と同様
の方法で二次電池用外装材料を得た。Comparative Example 2 An exterior material for a secondary battery was obtained in the same manner as in Example 2, except that the chromium conversion coating was not formed.
【００２２】比較例３
クロム化成処理皮膜を形成せずに、以下のようなジルコ
ニウム化成処理皮膜を形成した他は、実施例１と同様の
方法で二次電池用外装材料を得た。ジルコニウム化成処
理皮膜は、アンモニウムジルコニウムカーボネートとポ
リアクリル酸を主成分とする水溶液（ジルコニウム処理
液）を、アルミニウム箔両面に均一に塗布し、１５０℃
で１５秒間の条件で乾燥して、得られたものである。な
お、ジルコニウム化成処理皮膜中におけるジルコニウム
含有量は、２０ｍｇ／ｍ2とした。Comparative Example 3 An exterior material for a secondary battery was obtained in the same manner as in Example 1 except that the zirconium chemical conversion coating as described below was formed without forming the chromium chemical conversion coating. The zirconium chemical conversion coating film is obtained by uniformly applying an aqueous solution (zirconium processing solution) containing ammonium zirconium carbonate and polyacrylic acid as main components to both surfaces of the aluminum foil at 150 ° C.
It was obtained by drying under conditions of 15 seconds. The zirconium content in the zirconium chemical conversion coating was 20 mg / m 2 .
【００２３】比較例４
クロム化成処理皮膜を形成せずに、比較例３と同一のジ
ルコニウム化成処理皮膜を形成した他は、実施例２と同
様の方法で二次電池用外装材料を得た。Comparative Example 4 An exterior material for a secondary battery was obtained in the same manner as in Example 2, except that the same zirconium chemical conversion coating as in Comparative Example 3 was formed without forming the chromium chemical conversion coating.
【００２４】比較例５
クロム化成処理皮膜を形成せずに、アルミニウム箔表面
に脱脂処理及びエッチング処理を施した他は、実施例１
と同様の方法で二次電池用外装材料を得た。Comparative Example 5 Example 1 was repeated except that the aluminum foil surface was subjected to degreasing treatment and etching treatment without forming a chromium conversion coating.
A packaging material for a secondary battery was obtained by the same method as described in.
【００２５】比較例６
クロム化成処理皮膜を形成せずに、アルミニウム箔表面
に脱脂処理及びエッチング処理を施した他は、実施例２
と同様の方法で二次電池用外装材料を得た。Comparative Example 6 Example 2 was repeated except that the aluminum foil surface was subjected to degreasing treatment and etching treatment without forming a chromium conversion coating.
A packaging material for a secondary battery was obtained by the same method as described in.
【００２６】実施例１、２及び比較例１〜６に係る方法
で得られた各二次電池用外装材料から、巾１５ｍｍの短
冊片２枚を裁断し、試験片を得た。１個の試験片につい
ては、二次電池用外装材料製造後直ちに、金属箔と３層
共押出フィルム間、又は金属箔と無水マレイン酸変成ポ
リプロピレンフィルム単層間の剥離強度を測定した。そ
の結果を、表１の初期剥離強度（ｋｇ／１５ｍｍ巾）と
して示した。Two strips having a width of 15 mm were cut from each of the secondary battery outer packaging materials obtained by the methods according to Examples 1 and 2 and Comparative Examples 1 to 6 to obtain test pieces. For one test piece, the peel strength between the metal foil and the three-layer coextruded film or between the metal foil and the maleic anhydride-modified polypropylene film single layer was measured immediately after the production of the secondary battery exterior material. The results are shown as the initial peel strength (kg / 15 mm width) in Table 1.
【００２７】他の１個の試験片については、エチレンカ
ーボネート５０重量部、ジエチルカーボネート４０重量
部、六フッ化リン酸リチウム（ＬｉＰＦ6）１０重量部
からなる電解液に浸漬し、温度２０℃、湿度５０％ＲＨ
の雰囲気下で開放状態のまま、２４時間放置した。その
後、この試験片の金属箔と３層共押出フィルム間、又は
金属箔と無水マレイン酸変成ポリプロピレンフィルム単
層間の剥離強度を測定した。その結果を、表１の２４時
間後の剥離強度（ｋｇ／１５ｍｍ巾）として示した。Another test piece was immersed in an electrolytic solution containing 50 parts by weight of ethylene carbonate, 40 parts by weight of diethyl carbonate, and 10 parts by weight of lithium hexafluorophosphate (LiPF 6 ) at a temperature of 20 ° C. Humidity 50% RH
It was left for 24 hours in an open state under the above atmosphere. Then, the peel strength between the metal foil and the three-layer coextruded film of this test piece, or between the metal foil and the maleic anhydride modified polypropylene film single layer was measured. The results are shown in Table 1 as the peel strength after 24 hours (kg / 15 mm width).
【００２８】また、実施例１、２及び比較例１〜６に係
る方法で得られた各二次電池用外装材料から、縦９０ｍ
ｍで横５０ｍｍの大きさの四辺形状片２枚を裁断した。
そして、熱封緘層同士が当接するようにして、２枚の四
辺形状片を積層し、３方の端部を巾５ｍｍで熱封緘し、
四辺形状袋を作成した。熱封緘の条件は、温度２００
℃、圧力２ｋｇ／ｃｍ2、時間１秒間とした。そして、
この袋の口から、エチレンカーボネート５０重量部、ジ
エチルカーボネート４０重量部、六フッ化リン酸リチウ
ム（ＬｉＰＦ6）１０重量部からなる電解液を注入し
た。最後に袋の口を、前の条件と同一の条件で熱封緘
し、試験体を得た。なお、このような試験体を、各実施
例及び比較例につき、２個準備した。Further, from the exterior materials for secondary batteries obtained by the methods according to Examples 1 and 2 and Comparative Examples 1 to 6, a length of 90 m was obtained.
Two quadrilateral pieces each having a size of 50 mm and a width of 50 mm were cut.
Then, two quadrilateral pieces are laminated so that the heat sealing layers are in contact with each other, and the three ends are heat sealed with a width of 5 mm,
A quadrilateral bag was created. The condition for heat sealing is a temperature of 200.
° C., the pressure 2 kg / cm 2, and a time of 1 second. And
From the mouth of this bag, an electrolytic solution containing 50 parts by weight of ethylene carbonate, 40 parts by weight of diethyl carbonate, and 10 parts by weight of lithium hexafluorophosphate (LiPF 6 ) was injected. Finally, the mouth of the bag was heat-sealed under the same conditions as the previous conditions to obtain a test body. Two such test bodies were prepared for each example and comparative example.
【００２９】１個の試験体については、温度６０℃で湿
度９０％ＲＨの雰囲気下で２０日間放置した後、この試
験体から、巾１５ｍｍの短冊片を裁断し、金属箔と３層
共押出フィルム間、又は金属箔と無水マレイン酸変成ポ
リプロピレンフィルム単層間の剥離強度を測定した。そ
の結果を、表１の２０日間後の剥離強度（ｋｇ／１５ｍ
ｍ巾）として示した。One test piece was allowed to stand in an atmosphere of a temperature of 60 ° C. and a humidity of 90% RH for 20 days, and then a strip of 15 mm in width was cut from this test piece, and a metal foil and three layers were coextruded. The peel strength between the films or between the metal foil and the maleic anhydride modified polypropylene film single layer was measured. The results are shown in Table 1 for peel strength after 20 days (kg / 15 m
m width).
【００３０】他の１個の試験体については、温度８５℃
で湿度９０％ＲＨの雰囲気下で７日間放置した後、この
試験体から、巾１５ｍｍの短冊片を裁断し、金属箔と３
層共押出フィルム間、又は金属箔と無水マレイン酸変成
ポリプロピレンフィルム単層間の剥離強度を測定した。
その結果を、表１の７日間後の剥離強度（ｋｇ／１５ｍ
ｍ巾）として示した。For the other test piece, the temperature was 85 ° C.
After leaving it in an atmosphere of 90% RH for 7 days, a strip with a width of 15 mm was cut from this test piece, and cut with a metal foil.
The peel strength between the layer coextruded films or between the metal foil and the maleic anhydride modified polypropylene film single layer was measured.
The results are shown in Table 1 for peel strength after 7 days (kg / 15 m
m width).
【００３１】[0031]
【表１】
なお、剥離強度の試験方法は、剥離角度Ｔピールで剥離
速度２００ｍｍ／ｍｉｎの条件で測定した。また、表１
中、剥離強度が０．００ｋｇ／１５ｍｍ巾とあるのは、
既に剥離試験に供する前にデラミ（剥離）が生じている
ものである。[Table 1] In addition, the peeling strength test method was performed under the conditions of a peeling angle T peel and a peeling speed of 200 mm / min. Also, Table 1
In the middle, the peel strength is 0.00kg / 15mm width,
Delamination (peeling) has already occurred before being subjected to the peeling test.
【００３２】実施例１、２及び比較例１〜６の結果を対
比すれば明らかなとおり、クロメート処理によってクロ
ム化成処理皮膜を設けた金属箔を用いれば、処理を施し
ていない金属箔、ジルコニウム処理によってジルコニウ
ム化成処理皮膜を設けた金属箔、及びエッチング処理を
施した金属箔に比べて、六フッ化リン酸リチウム（Ｌｉ
ＰＦ6）を含む電解液と接触しても、熱封緘層と金属箔
（外装材本体）とが剥離しにくいことが分かる。従っ
て、実施例に係る二次電池用外装材料を用いて二次電池
を得れば、比較例に係るものを用いた場合に比べて、使
用中等に電解液の漏れが生じにくいことが分かる。As is clear from comparison between the results of Examples 1 and 2 and Comparative Examples 1 to 6, when the metal foil provided with the chromium conversion coating by the chromate treatment is used, the untreated metal foil and the zirconium treatment are used. In comparison with the metal foil provided with the zirconium chemical conversion treatment film and the metal foil subjected to the etching treatment, lithium hexafluorophosphate (Li
It can be seen that the heat-sealing layer and the metal foil (main body of exterior material) are not easily peeled off even if they are brought into contact with the electrolytic solution containing PF 6 ). Therefore, it can be seen that when a secondary battery is obtained using the secondary battery outer packaging material according to the example, the electrolyte does not easily leak during use as compared with the case where the comparative example is used.
【００３３】[0033]
【発明の効果】以上説明したように、本発明に係る二次
電池用外装材料を用いて、二次電池を得れば、熱封緘層
と外装材本体とが剥離しにくく、封入された電解液の液
漏れが生じにくくなる。従って、二次電池が組み込まれ
たエレクトロニクス機器等に、液漏れによる障害の発生
を防止しうるという格別顕著な効果を奏するものであ
る。As described above, when a secondary battery is obtained by using the secondary battery outer packaging material according to the present invention, the heat sealing layer and the outer packaging material main body do not easily peel off, and the enclosed electrolytic Liquid leakage is less likely to occur. Therefore, it has an especially remarkable effect that it is possible to prevent the occurrence of troubles due to liquid leakage in electronic devices and the like in which the secondary battery is incorporated.
【図１】シート状で薄型のポリマーリチウムイオン二次
電池の内部構造の一例を示した模式的断面図である。FIG. 1 is a schematic cross-sectional view showing an example of the internal structure of a thin sheet-shaped polymer lithium ion secondary battery.
【図２】二次電池の外装材の一般例を示した模式的断面
図である。FIG. 2 is a schematic cross-sectional view showing a general example of an exterior material for a secondary battery.
【図３】本発明の一例に係る二次電池用外装材料の模式
的断面図である。FIG. 3 is a schematic cross-sectional view of an exterior material for a secondary battery according to an example of the present invention.
【図４】本発明の他の例に係る二次電池用外装材料の模
式的断面図である。FIG. 4 is a schematic cross-sectional view of a packaging material for a secondary battery according to another example of the present invention.
【符号の説明】
１ 外装材
９ 熱封緘層（無水マレイン酸変成ポリプロピレンフ
ィルム）
９’ 無水マレイン酸変成ポリプロピレンフィルム
１０ 金属箔
１１ 金属箔本体
１２ クロム化成処理皮膜
１３ 接着性皮膜
１４ ポリオレフィン系フィルム
１５ ポリプロピレンフィルム[Explanation of Codes] 1 Exterior material 9 Heat sealing layer (maleic anhydride modified polypropylene film) 9'Maleic anhydride modified polypropylene film 10 Metal foil 11 Metal foil body 12 Chromium conversion coating 13 Adhesive coating 14 Polyolefin film 15 Polypropylene the film
───────────────────────────────────────────────────── フロントページの続き (56)参考文献 特開 平11−67166（ＪＰ，Ａ) 特開 平６−99542（ＪＰ，Ａ) 特開 平６−302305（ＪＰ，Ａ) 特開 平10−312788（ＪＰ，Ａ) 特開 平１−235637（ＪＰ，Ａ) (58)調査した分野(Int.Cl.7，ＤＢ名) H01M 2/02 ─────────────────────────────────────────────────── ─── Continuation of the front page (56) Reference JP-A-11-67166 (JP, A) JP-A-6-99542 (JP, A) JP-A-6-302305 (JP, A) JP-A-10- 312788 (JP, A) JP-A-1-235637 (JP, A) (58) Fields investigated (Int.Cl. 7 , DB name) H01M 2/02
Claims (6)
も片面全面にクロメート処理により形成されたクロム化
成処理皮膜とからなる金属箔の、該クロム化成処理皮膜
側全面に酸変成ポリオレフィンフィルムよりなる熱封緘
層が設けられていることを特徴とする二次電池用外装材
料。1. A metal foil comprising a metal foil main body and a chromium chemical conversion coating formed by chromate treatment on at least one entire surface of the metal foil main body, and an acid-modified polyolefin film on the entire surface of the chromium chemical conversion coating. An exterior material for a secondary battery, which is provided with a heat-sealing layer.
施されたアルミニウム箔である請求項１記載の二次電池
用外装材料。2. The exterior material for a secondary battery according to claim 1, wherein the metal foil body is an aluminum foil whose surface is anodized.
変成ポリオレフィンである請求項１又は２記載の二次電
池用外装材料。3. The exterior material for a secondary battery according to claim 1, wherein the acid-modified polyolefin is a maleic anhydride-modified polyolefin.
も片面全面にクロメート処理により形成されたクロム化
成処理皮膜とからなる金属箔の、該クロム化成処理皮膜
面全面に、酸変成ポリオレフィンを固形分とするオルガ
ノゾルを塗布した後、該オルガノゾルを乾燥して接着性
皮膜を形成せしめ、次いで、該オルガノゾル中の酸変成
ポリオレフィンと同種の酸変成ポリオレフィンフィルム
を該接着性皮膜に圧着して、該金属箔と該酸変成ポリオ
レフィンフィルムとを貼着し、該酸変成ポリオレフィン
フィルムを熱封緘層とすることを特徴とする二次電池用
外装材料の製造方法。4. A metal foil body, a metal foil made of a chromium chemical conversion coating formed by at least one side entire surface chromate treatment of the metal foil body, to the chromium chemical conversion coating the entire surface, a solid acid-modified polyolefin After coating the organosol to be used as a component, the organosol is dried to form an adhesive film, and then the acid-modified polyolefin film of the same kind as the acid-modified polyolefin in the organosol is pressure-bonded to the adhesive film to form the metal. A method for producing a packaging material for a secondary battery, comprising laminating a foil and the acid-modified polyolefin film, and using the acid-modified polyolefin film as a heat-sealing layer.
も片面全面にクロメート処理により形成されたクロム化
成処理皮膜とからなる金属箔の、該クロム化成処理皮膜
面全面に、酸変成ポリオレフィンを固形分とするオルガ
ノゾルを塗布した後、該オルガノゾルを乾燥して接着性
皮膜を形成せしめ、次いで、該オルガノゾル中の酸変成
ポリオレフィンと同種の酸変成ポリオレフィンフィルム
を両面に備えたポリオレフィン系フィルムの該酸変成ポ
リオレフィンフィルムの一方と該接着性皮膜とを圧着し
て、該金属箔と該ポリオレフィン系フィルムとを貼着
し、該酸変成ポリオレフィンフィルムの他方を熱封緘層
とすることを特徴とする二次電池用外装材料の製造方
法。5. A metal foil body, a metal foil made of a chromium chemical conversion coating formed by at least one side entire surface chromate treatment of the metal foil body, to the chromium chemical conversion coating the entire surface, a solid acid-modified polyolefin After coating the organosol to be used as a component, the organosol is dried to form an adhesive film, and then the acid-modified polyolefin film having the same acid-modified polyolefin film as the acid-modified polyolefin in the organosol on both sides thereof. A secondary battery characterized in that one side of the polyolefin film and the adhesive film are pressure-bonded to each other, the metal foil and the polyolefin-based film are adhered to each other, and the other side of the acid-modified polyolefin film is a heat-sealing layer. For manufacturing exterior materials for automobiles.
変成ポリオレフィンである請求項４又は５記載の二次電
池用外装材料の製造方法。6. The method for producing a packaging material for a secondary battery according to claim 4, wherein the acid-modified polyolefin is a maleic anhydride-modified polyolefin.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP16748399A JP3496090B2 (en) | 1999-06-14 | 1999-06-14 | Exterior material for secondary battery and method of manufacturing the same |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP16748399A JP3496090B2 (en) | 1999-06-14 | 1999-06-14 | Exterior material for secondary battery and method of manufacturing the same |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JP2000357494A JP2000357494A (en) | 2000-12-26 |
| JP3496090B2 true JP3496090B2 (en) | 2004-02-09 |
Family
ID=15850530
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP16748399A Expired - Fee Related JP3496090B2 (en) | 1999-06-14 | 1999-06-14 | Exterior material for secondary battery and method of manufacturing the same |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3496090B2 (en) |
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- 1999-06-14 JP JP16748399A patent/JP3496090B2/en not_active Expired - Fee Related
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