JP3677270B2 - Method for producing lithium polymer secondary battery - Google Patents

Method for producing lithium polymer secondary battery Download PDF

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Publication number
JP3677270B2
JP3677270B2 JP2003007642A JP2003007642A JP3677270B2 JP 3677270 B2 JP3677270 B2 JP 3677270B2 JP 2003007642 A JP2003007642 A JP 2003007642A JP 2003007642 A JP2003007642 A JP 2003007642A JP 3677270 B2 JP3677270 B2 JP 3677270B2
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separation membrane
electrode plate
secondary battery
lithium polymer
negative electrode
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JP2004220943A (en
Inventor
ウー ハン，ソン
ジェ キム，ヨン
ハク リ，ジュー
チェン キム，ジョン
ホ ジン，スク
ヨル リ，カブ
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SAEHAN ENERTECH Inc
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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Description

【０００１】
【発明の属する技術分野】
本発明は、リチウムポリマー２次電池の製造方法に関し、さらに詳細には、正極、負極、分離膜を組合せる方式において、単位セルを回転軸として、その単位セルの外周に一定の引張力を保持しながら分離膜を巻取って製造するリチウムポリマー２次電池の製造方法に関する。
【０００２】
【従来の技術】
周知の如く、ノート型パーソナルコンピュータおよびセルラーホン(cellular phone)などのポータブル機器の急速な拡大に伴って高容量・高性能の再充電用２次電池の需要が急増している。現在、２次電池のリチウムイオンの吸蔵および放出可能な炭素材を活物質に使用した負極、構造変形によってリチウムイオンの充放電が可能なリチウム複合酸化物を用いた正極、リチウムイオンの媒介体に非水電解液を使用したリチウムイオン２次電池が開発され、広く使用されている。しかし、この種のイオン電池は、水分との反応性が大きく、熱的に不安定な過量の電解液を使用するため、安定性を信頼できなく、また、電池包装材として金属缶などを使用するため、エネルギー密度に劣り、電池形態の変化が不自由な問題がある。
【０００３】
これらの問題を補完するために提示された、高分子電解質を使用するリチウムポリマー２次電池は、液体電解質を使用するリチウムイオン２次電池に比べ、漏液が少なく電池形態が白由であり、エネルギー密度が高く、小型であり、軽量化および薄型化が可能であり、安全性に優れている（例えば、特許文献１参照。他多数の特許文献参照。）。
【０００４】
図１は、巻取り方法によるリチウムポリマー２次電池の製造方法を示す図であって、前記特許文献１でも採用している方法である。前記特許文献１ではジェリーロール型のものが開示されている。
【０００５】
これは、ジェリーロールを角形の缶に入れた後、その上にキャップをしレーザ融着でシーリングした構造を持っている。このとき、負極と正極はそれぞれ、銅薄板とアルミニウム薄板の両面に高分子結着剤、導電性粉末、そして各電極活物質の混合剤を塗布して製造し、通常、電極タップの取り付けのために未コーティング部位を残す。負極と正極の未コーティング部には通常、それぞれニッケルとアルミニウム材質の電極タップを取り付け、これを用いて両電極を電池の外部端子に連結する。このとき、未コーティング部に取り付けた電極タップの一つは、ジェリーロールが缶に挿入されるとき缶の底部や側面に付着され、もう一つはキャップに付着される。このような組合方式および構造から得られるメリットは、まず、巻取りのとき分離膜に加えられる張力によって正極と負極が物理的に均一に密着されており、また缶の壁によって物理的に圧着されているため、電気化学的反応によって電池が充電または放電されるとき、全体電極面が均一に活用されるということである。したがって、基本的に電池性能に優れるとともに、長期充放電サイクルに対しても高い性能が保持される。機械的な強度の大きい金属材質の缶の壁から得られる他のメリットは、その物理的圧着力によって缶内にジェリーロールを強く圧着して充填することができ、内部の変形力によって起こり得る厚さ変形を最小化できるという点であって、最終的な電池の単位体積あたりエネルギー密度の向上に大いに寄与する。また、電池缶とキャップが完全に融着されて電池の内部と外部を完全に断絶させているため、電池内物質の漏れと電池外からの異物の内部浸透が防止される。
【０００６】
しかし、前記巻取り方法によって作製されたリチウムポリマー２次電池は、巻取りのときに分離膜に加えられる張力が一定ではないため、図１に示すように巻かれた状態が実際には完璧に平坦でない変形された楕円形状に近くなり、角形の缶内に隙間なく嵌められない。したがって、セルの両端部と中央部には集中される応力差が生じてしまうので、長期にわたる充放電過程において電池の寿命が短縮される問題が起こる。
【０００７】
また、特許文献２には、複数の積層された電極が一定面積を保持しながら積層(stacking)されるジグザグスタッキング(Zig-Zag Stacking)方法が示されている。これによって製作されたセルは平面上に積層されたものなので、原理的に応力の差が発生しない。しかしながら、この方式では、図２に示すように、積層工程の上で分離膜の折り返し部分において必然的に極板と分離膜との間に隙間が発生する。その結果、長期問の充放電過程において極板と分離膜との隙間によって両端部（折り返し部分）が膨らむ問題が生じ、結果として電池寿命の短縮を招くという問題があった。
【０００８】
【特許文献１】
米国特許第６，４６８，６９３号明細書
【特許文献２】
米国特許第４，０４８，３９７号明細書
【０００９】
【発明が解決しようとする課題】
したがって、本発明は、先に述べた巻取り方式とジグザグスタッキング方式で生じてきた問題点を解決するために案出されたものであり、特に、電極と分離膜との隙間を最小化し、極板全面の応力を均一にすることによって電池の寿命が延びるようにしたリチウムポリマー２次電池の製造方法を提供することにその目的がある。
【００１０】
【課題を解決するための手段】
前記目的を達成するために、本発明は、一定（所定）の正極板および負極板を分離膜に密着させた単位セルを回転軸で回転させ、その単位セルの外周に、一定の引張力で保持される分離膜を巻き付けて組合せることを特徴とするリチウムポリマー２次電池の製造方法を提供する。
【００１１】
【発明の実施の形態】
以下、添付図面を参照しつつ本発明を詳細に説明する。本発明によるリチウムポリマー２次電池の組合方式は、図３（Ａ）に示すように、正極活物質が塗布、乾燥してある正極板２、負極活物質が塗布、乾燥してある負極板３、および前記両電極２、３を絶縁する特性を有するポリオレフィンからなる分離膜１で構成される。本発明は、前記構造の単位セルを、図３（Ｂ）（Ｃ）に示すように、回転させながら一定の引張力で保持される分離膜１も巻いて積層する方式であって、その完成した一例を図４に示す。
【００１２】
このとき、一定の引張力で保持される分離膜１の引張力は、およそ０．３〜５．０kgf/cm2の範囲が好ましいが、０．３kgf/cm2未満では引張力が弱く隙間が生じやすく、５．０kgf/cm2を超えると、引張力が強すぎて単位セルを回転させ難くなり、作業性に問題が生じる。
【００１３】
以下、実施例および比較例を上げて本発明をさらに具体的に説明する。
【００１４】
【実施例１】
リチウムポリマー2次電池の規格は１．３Ah級であって、正極板２はアルミホイルにLiCoO2を薄膜コーティングし、負極板は銅ホイルにグラファイト(graphite)を薄膜コーティングして製造された電極である。このとき、正極板２は横４６．０mm、縦５０．４ｍｍに、負極板３は横長４６．６ｍｍ、縦長５２．０mmに、分離膜１の幅は５３．５mmにパンチングした。そして、図３（Ａ）のような過程によって正極板２に分離膜１を先に巻いて固定して単位セルを形成した後、図３（Ｂ）（Ｃ）のように、分離膜１を１．５kgf/cm2の一定な引張力を保持しながら前記単位セルを回転させ、分離膜１を挟んで正極板２と負極板３を交互に配置して積層した。この方法によって組合せた後、アルミニウムパウチ内に挿入した後、一面を除いた各面をシーリングし、続いてシーリングしなかった部位を通じて１Ｍ（mol） LiPF8／ＥＣ：ＰＣ：ＥＭＣ（３０：１０：６０）４．７ｇを注入し、真空下でシーリングした後、電解質を十分に電極に含浸させた。ここで、LiPF8はLitium Hexafluorophosphate、ＥＣはEthylene Carbonate、ＰＣはPropylene Carbonate、ＥＭＣはEthylmethyl Carbonateである。
【００１５】
【比較例１】
図１のような巻取り方式で組合せたことを除いては実施例１と同様にして行った。
【００１６】
【比較例２】
図２のようなジグザクスタッキング方式で組合せたことを除いては実施例１と同様にして行った。
【００１７】
前記実施例および比較例で作製された電池を下記の方法で充電し、電池の寿命を評価し、その結果を表１に表した。
【００１８】
（充放電方法および電池寿命の評価）
前記実施例および比較例によって製造された電池を電池設計容量に対してそれぞれ、０．０５Ｃ（capacity）で３．１５Ｖまで、０．２Ｃ（capacity）で４．２Ｖまで２段階に初期充電をし、この電池を、安定化過程を経た後４．２Ｖまで１Ｃ（capacity）で定電圧・定電流で充電した後、３．０Ｖまで１．０Ｃ（capacity）で放電し、電池寿命評価は充放電テスト機（ＴＯＳＣＡＴ−３１００Ｕ）で常温で測定した。
【００１９】
【表１】

Figure 0003677270
【００２０】
【発明の効果】
以上の実施例および比較例から分かるように、本発明によるリチウムポリマー２次電池は、電池全面に均一な応力が加えられ、分離膜と電極との隙間―を最小化して長期問の充放電過程で容量保持率が高く表れるので、電池の寿命的特性が向上する有用性が得られる。
【図面の簡単な説明】
【図１】 巻取り方法によるリチウムポリマー２次電池製造法の例示図。
【図２】 ジグザクスタッキング方法によるリチウムポリマー２次電池製造法の例示図。
【図３】 本発明によるリチウムポリマー２次電池製造法の例示図であって、（Ａ）は正極板の外周に分離膜を巻く工程を示す図、（Ｂ）は分離膜が巻かれた正極板に負極板を積層する工程を示す図、（Ｃ）は負極板の外周に分離膜を巻く工程を示す図。
【図４】 本発明によって製造されたリチウムポリマー２次電池の構成図。
【符号の説明】
１ 分離膜
２ 正極板
３ 負極板[0001]
BACKGROUND OF THE INVENTION
The present invention relates to a method for manufacturing a lithium polymer secondary battery, and more particularly, in a method in which a positive electrode, a negative electrode, and a separation membrane are combined, a unit cell is used as a rotation axis, and a constant tensile force is maintained on the outer periphery of the unit cell. The present invention relates to a method for producing a lithium polymer secondary battery in which a separation membrane is wound up and produced.
[0002]
[Prior art]
As is well known, with the rapid expansion of portable devices such as notebook personal computers and cellular phones, the demand for high-capacity, high-performance rechargeable secondary batteries has increased rapidly. Currently, a negative electrode using a carbon material capable of occluding and releasing lithium ions in a secondary battery as an active material, a positive electrode using a lithium composite oxide capable of charging and discharging lithium ions by structural deformation, and a lithium ion mediator Lithium ion secondary batteries using non-aqueous electrolytes have been developed and are widely used. However, this type of ion battery uses a large amount of electrolyte that is highly reactive with moisture and is thermally unstable, so the stability is unreliable and metal cans are used as battery packaging materials. Therefore, there is a problem that the energy density is inferior and the change in battery form is inconvenient.
[0003]
The lithium polymer secondary battery using a polymer electrolyte, which has been proposed to compensate for these problems, has less leakage and a white battery form than a lithium ion secondary battery using a liquid electrolyte. The energy density is high, the size is small, the weight can be reduced and the thickness can be reduced, and the safety is excellent (see, for example, Patent Document 1 and many other patent documents).
[0004]
FIG. 1 is a diagram showing a method of manufacturing a lithium polymer secondary battery by a winding method, and is also a method adopted in Patent Document 1. In Patent Document 1, a jelly roll type is disclosed.
[0005]
This has a structure in which a jelly roll is put in a square can, and then a cap is placed thereon and sealed by laser fusion. At this time, the negative electrode and the positive electrode are respectively manufactured by applying a polymer binder, a conductive powder, and a mixture of each electrode active material on both sides of a copper thin plate and an aluminum thin plate. Leave an uncoated site. Usually, nickel and aluminum electrode taps are attached to the uncoated portions of the negative electrode and the positive electrode, respectively, and both electrodes are connected to the external terminals of the battery. At this time, one of the electrode taps attached to the uncoated portion is attached to the bottom or side of the can when the jelly roll is inserted into the can, and the other is attached to the cap. The merit obtained from such a combination system and structure is that the positive electrode and the negative electrode are physically and uniformly adhered to each other by the tension applied to the separation membrane at the time of winding, and is physically pressed by the wall of the can. Therefore, when the battery is charged or discharged by an electrochemical reaction, the entire electrode surface is utilized uniformly. Therefore, the battery performance is basically excellent and high performance is maintained even for a long-term charge / discharge cycle. Another merit that can be obtained from the wall of a metal can with high mechanical strength is that the jelly roll can be strongly pressed and filled into the can by its physical pressing force, which can be caused by internal deformation force. This is that the deformation can be minimized, which greatly contributes to the improvement of the energy density per unit volume of the final battery. Further, since the battery can and the cap are completely fused to completely disconnect the inside and outside of the battery, leakage of the substance inside the battery and internal penetration of foreign matter from outside the battery are prevented.
[0006]
However, in the lithium polymer secondary battery manufactured by the winding method, since the tension applied to the separation membrane during winding is not constant, the wound state as shown in FIG. It becomes close to a deformed elliptical shape that is not flat, and cannot be fitted into a square can without a gap. Therefore, a concentrated stress difference is generated between the both ends and the center of the cell, which causes a problem that the battery life is shortened in a long-time charge / discharge process.
[0007]
Patent Document 2 discloses a Zig-Zag Stacking method in which a plurality of stacked electrodes are stacked while maintaining a certain area. Since the cells manufactured in this way are stacked on a plane, in principle there is no difference in stress. However, in this method, as shown in FIG. 2, a gap is inevitably generated between the electrode plate and the separation membrane at the folded portion of the separation membrane in the stacking process. As a result, there is a problem that both end portions (folded portions) swell due to a gap between the electrode plate and the separation membrane in a long-term charging / discharging process, resulting in a reduction in battery life.
[0008]
[Patent Document 1]
US Pat. No. 6,468,693 [Patent Document 2]
US Pat. No. 4,048,397 Specification
[Problems to be solved by the invention]
Therefore, the present invention has been devised to solve the problems caused by the winding method and the zigzag stacking method described above, and in particular, the gap between the electrode and the separation membrane is minimized, It is an object of the present invention to provide a method for producing a lithium polymer secondary battery in which the life of the battery is extended by making the stress on the entire plate uniform.
[0010]
[Means for Solving the Problems]
In order to achieve the above object, the present invention is to rotate a unit cell having a fixed (predetermined) positive electrode plate and a negative electrode plate in close contact with a separation membrane on a rotating shaft, and to the outer periphery of the unit cell with a constant tensile force. Provided is a method for producing a lithium polymer secondary battery, wherein a separation membrane to be held is wound and combined.
[0011]
DETAILED DESCRIPTION OF THE INVENTION
Hereinafter, the present invention will be described in detail with reference to the accompanying drawings. As shown in FIG. 3A, the combination system of the lithium polymer secondary battery according to the present invention includes a positive electrode plate 2 on which a positive electrode active material is applied and dried, and a negative electrode plate 3 on which a negative electrode active material is applied and dried. And a separation membrane 1 made of polyolefin having the property of insulating the electrodes 2 and 3. The present invention is a method of winding and laminating the separation cell 1 held by a constant tensile force while rotating the unit cell having the above structure as shown in FIGS. 3B and 3C. An example of this is shown in FIG.
[0012]
At this time, the tensile force of the separation membrane 1 held at a constant tensile force is preferably in the range of about 0.3 to 5.0 kgf / cm 2 , but if it is less than 0.3 kgf / cm 2 , the tensile force is weak and there is a gap. If it exceeds 5.0 kgf / cm 2 , the tensile force is too strong and it becomes difficult to rotate the unit cell, causing a problem in workability.
[0013]
Hereinafter, the present invention will be described more specifically with reference to examples and comparative examples.
[0014]
[Example 1]
The standard of the lithium polymer secondary battery is 1.3 Ah class. The positive electrode plate 2 is an electrode manufactured by thin film coating of LiCoO 2 on aluminum foil and thin film coating of graphite (graphite) on copper foil. is there. At this time, the positive electrode plate 2 was punched to a width of 46.0 mm and a vertical length of 50.4 mm, the negative electrode plate 3 was punched to a horizontal length of 46.6 mm and a vertical length of 52.0 mm, and the width of the separation membrane 1 was punched to 53.5 mm. Then, after the separation membrane 1 is wound around and fixed to the positive electrode plate 2 by a process as shown in FIG. 3A to form a unit cell, the separation membrane 1 is formed as shown in FIGS. The unit cell was rotated while maintaining a constant tensile force of 1.5 kgf / cm 2 , and the positive electrode plate 2 and the negative electrode plate 3 were alternately arranged and laminated with the separation membrane 1 interposed therebetween. After combining by this method, after inserting into an aluminum pouch, each side except one side was sealed, and then 1M (mol) LiPF 8 / EC: PC: EMC (30:10: 60) After 4.7 g was injected and sealed under vacuum, the electrode was sufficiently impregnated with the electrolyte. Here, LiPF 8 is Litium Hexafluorophosphate, EC is Ethylene Carbonate, PC is Propylene Carbonate, and EMC is Ethylmethyl Carbonate.
[0015]
[Comparative Example 1]
The same procedure as in Example 1 was performed except that the winding method as shown in FIG.
[0016]
[Comparative Example 2]
This was performed in the same manner as in Example 1 except that they were combined in a zigzag stacking system as shown in FIG.
[0017]
The batteries produced in the examples and comparative examples were charged by the following method, the battery life was evaluated, and the results are shown in Table 1.
[0018]
(Evaluation of charge / discharge method and battery life)
The batteries manufactured according to the examples and comparative examples were initially charged in two stages with respect to the battery design capacity up to 3.15 V at 0.05 C (capacity) and 4.2 V at 0.2 C (capacity), respectively. After the stabilization process, the battery was charged at a constant voltage / constant current up to 4.2V at 1C (capacity), and then discharged at 1.0C (capacity) up to 3.0V. It measured at normal temperature with the test machine (TOSCAT-3100U).
[0019]
[Table 1]
Figure 0003677270
[0020]
【The invention's effect】
As can be seen from the above examples and comparative examples, the lithium polymer secondary battery according to the present invention is applied with a uniform stress on the entire surface of the battery, minimizing the gap between the separation membrane and the electrode, and thus a long-term charge / discharge process. As a result, the capacity retention ratio is high, and usefulness for improving the life characteristics of the battery can be obtained.
[Brief description of the drawings]
FIG. 1 is an exemplary view of a method for producing a lithium polymer secondary battery by a winding method.
FIG. 2 is an exemplary diagram of a method for producing a lithium polymer secondary battery by a zigzag stacking method.
FIG. 3 is an exemplary view of a method for producing a lithium polymer secondary battery according to the present invention, in which (A) shows a process of winding a separation membrane around the outer periphery of the positive electrode plate, and (B) is a positive electrode on which the separation membrane is wound. The figure which shows the process of laminating | stacking a negative electrode plate on a board, (C) is a figure which shows the process of winding a separation membrane around the outer periphery of a negative electrode plate.
FIG. 4 is a configuration diagram of a lithium polymer secondary battery manufactured according to the present invention.
[Explanation of symbols]
1 Separation membrane 2 Positive electrode plate 3 Negative electrode plate

Claims (2)

一枚づつ所定寸法である正極板と負極板が分離膜を挟んで配置された単位セルを回転軸にして回転させて、その外周に一定の引張力で保持された分離膜を巻き付けながら、巻き付けられた分離膜の外側に所定寸法の正極板と負極板を交互に配置し、配置された正極板、負極板の外側に前記分離膜を巻き付けて、正極板と負極板を分離膜を挟んで絶縁して積層することを特徴とするリチウムポリマー２次電池の製造方法。Positive and negative electrode plates are one by one predetermined dimension is rotated by the rotation axis arranged unit cells across the separation membrane, while winding the separation membrane, which is held at a constant tension on the outer periphery thereof, wound A positive electrode plate and a negative electrode plate having predetermined dimensions are alternately arranged outside the separation membrane, the separation membrane is wound around the arranged positive electrode plate and the negative electrode plate , and the positive electrode plate and the negative electrode plate are sandwiched between the separation membranes. A method for producing a lithium polymer secondary battery, wherein the layers are insulated and laminated . 前記分離膜の引張力は０．３〜５．０kgf/cm2の範囲にあることを特徴とする請求項１記載のリチウムポリマー２次電池の製造方法。 2. The method of manufacturing a lithium polymer secondary battery according to claim 1, wherein the separation membrane has a tensile force in the range of 0.3 to 5.0 kgf / cm < 2 >.
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