JPH05290886A - Layered type lithium secondary battery - Google Patents
Layered type lithium secondary batteryInfo
- Publication number
- JPH05290886A JPH05290886A JP4088812A JP8881292A JPH05290886A JP H05290886 A JPH05290886 A JP H05290886A JP 4088812 A JP4088812 A JP 4088812A JP 8881292 A JP8881292 A JP 8881292A JP H05290886 A JPH05290886 A JP H05290886A
- Authority
- JP
- Japan
- Prior art keywords
- secondary battery
- negative electrode
- lithium
- lithium secondary
- laminated
- 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- Withdrawn
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
-
- 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
Landscapes
- Secondary Cells (AREA)
Abstract
Description
【０００１】[0001]
【産業上の利用分野】この発明は、リチウム二次電池に
関し、特に負極の形状安定性に関する改良により、寿命
が引き伸ばされた積層型リチウム二次電池に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a lithium secondary battery, and more particularly to a laminated lithium secondary battery whose life is extended by improving the shape stability of a negative electrode.
【０００２】[0002]
【従来の技術および発明が解決しようとする課題】リチ
ウムを負極活物質として用いる二次電池は、高エネルギ
密度を有する次代の二次電池として期待されている。こ
のリチウム二次電池では、放電時にリチウムがイオンと
なって負極から放出される一方、充電時にリチウムイオ
ンがリチウムとなって負極上に析出する。2. Description of the Related Art A secondary battery using lithium as a negative electrode active material is expected as a next-generation secondary battery having a high energy density. In this lithium secondary battery, lithium ions become ions from the negative electrode during discharging, while lithium ions become lithium and deposit on the negative electrode during charging.
【０００３】従来の二次電池は、充電に際してリチウム
が負極上に粒状または針状に析出する傾向があった。こ
のような析出のため、充放電を繰返すと負極の脱落が起
こり、電池容量が低下した。その結果、電池の寿命は短
くなった。また、リチウムの針状析出物は、隔膜を貫い
て正極に達し、内部短絡を引起すことがあった。In a conventional secondary battery, lithium tends to be deposited on the negative electrode in the form of particles or needles during charging. Due to such precipitation, the negative electrode came off when the charge and discharge were repeated, and the battery capacity decreased. As a result, the battery life was shortened. Further, the acicular lithium deposit may penetrate the diaphragm and reach the positive electrode, causing an internal short circuit.
【０００４】このような事態をさけるため、たとえば、
負極にリチウム合金を用いてリチウムの粒状・針状析出
を抑制し、電池の寿命を伸ばす方法が開示されている
（特開昭５９−１３００７４および特開昭６３−２２４
１５０）。また、本発明者らは、リチウムまたはリチウ
ム合金を貫通孔を有する基板内部に保持することで、負
極の形状安定性を高めたリチウム二次電池用負極につい
て提案してきた。In order to avoid such a situation, for example,
A method has been disclosed in which a lithium alloy is used for the negative electrode to suppress granular or acicular deposition of lithium and prolong the life of the battery (JP-A-59-130074 and JP-A-63-224).
150). The present inventors have also proposed a negative electrode for a lithium secondary battery in which the shape stability of the negative electrode is improved by holding lithium or a lithium alloy inside a substrate having a through hole.
【０００５】このような対策により、負極の形状につい
てその安定性が高められ、その脱落を抑制して電池の寿
命を伸ばすことが可能である。しかしながら、これらの
技術を用いても、充放電サイクル数が増加するにつれ、
負極が脱落する傾向にあった。By taking such measures, it is possible to improve the stability of the shape of the negative electrode, prevent the negative electrode from falling off, and extend the life of the battery. However, even with these techniques, as the number of charge and discharge cycles increases,
The negative electrode tended to fall off.
【０００６】この発明の目的は、負極の形状安定化をさ
らに高めることによって、より長いサイクル寿命を有す
る積層型二次電池を提供することにある。An object of the present invention is to provide a laminated secondary battery having a longer cycle life by further improving the shape stabilization of the negative electrode.
【０００７】[0007]
【課題を解決するための手段】この発明に従う積層型リ
チウム系二次電池は、隔膜を間に挟んで正極と負極を重
ねた積層セルを有する電池において、積層セルにおいて
電極を積層した方向の厚みが一定に保持される構造を有
する。A laminated type lithium secondary battery according to the present invention is a battery having a laminated cell in which a positive electrode and a negative electrode are stacked with a diaphragm interposed therebetween, and a thickness in a direction in which electrodes are laminated in the laminated cell. Has a structure in which is held constant.
【０００８】積層セルにおいて電極を積層した方向の厚
みが一定に保持される構造には、たとえば、積層セルの
両端に当板を押付けボルト等により締付けた構造、積層
セルの両端をスプリングコイルまたは板バネ等で押付け
た構造、ならびに積層セルの両端にスプリング等をひっ
かけて積層セルを圧縮固定した構造などがあるが、これ
らの構造に限定されるものではなく、積層方向の厚みが
保持される構造であればどのような構造であっても構わ
ない。Examples of the structure in which the thickness of the laminated cell in which the electrodes are laminated are kept constant include, for example, a structure in which a contact plate is fastened to both ends of the laminated cell by pressing bolts or the like, or a spring coil or a plate is formed at both ends of the laminated cell. There are structures that are pressed by springs and the like, and structures where the laminated cells are compressed and fixed by hooking springs or the like on both ends of the laminated cell, but the structure is not limited to these structures, and the structure that maintains the thickness in the stacking direction. Any structure may be used as long as it is.
【０００９】この発明に従う電池において、正極には、
ポリアニリン、ポリピロール、ポリチオフェンおよびこ
れらの誘導体などの導電性高分子材料、バナジウム酸化
物、マンガン酸化物、コバルト酸化物、ニッケル酸化物
および鉄酸化物などの金属酸化物、これら金属酸化物に
リチウムが含有されたリチウム複合酸化物、マンガン、
コバルト、バナジウム、ニッケルおよび鉄などの複合酸
化物、またはこれら複合酸化物にリチウムが含有された
リチウム複合酸化物が好ましい材料として用いられる
が、これらに限定されるものではなく、リチウム二次電
池正極材料として適用できればどのようなものでも構わ
ない。一方、負極には、リチウム、リチウム合金、また
はカーボン−リチウム層間化合物などが好ましい材料と
して用いられる。In the battery according to the present invention, the positive electrode is
Conductive polymer materials such as polyaniline, polypyrrole, polythiophene and their derivatives, metal oxides such as vanadium oxide, manganese oxide, cobalt oxide, nickel oxide and iron oxide, and lithium contained in these metal oxides Lithium composite oxide, manganese,
A composite oxide of cobalt, vanadium, nickel and iron, or a lithium composite oxide containing lithium in these composite oxides is used as a preferable material, but is not limited to these, and a lithium secondary battery positive electrode Any material may be used as long as it can be applied as a material. On the other hand, for the negative electrode, lithium, a lithium alloy, a carbon-lithium intercalation compound, or the like is used as a preferable material.
【００１０】この発明に従う積層セルでは、通常、正
極、隔膜、負極の順でこれらが重ねられるが、積層順序
は特に限定されず、たとえば、隔膜、負極、隔膜、正極
…の順、または負極、隔膜、正極、隔膜…の順でも問題
はない。さらに、この発明において、正極、隔膜および
負極の積層数は任意であり、特に限定されるものではな
い。In the laminated cell according to the present invention, the positive electrode, the diaphragm, and the negative electrode are usually stacked in this order, but the stacking order is not particularly limited. For example, the diaphragm, the negative electrode, the diaphragm, the positive electrode, or the negative electrode. There is no problem in the order of diaphragm, positive electrode, diaphragm ... Further, in the present invention, the number of laminated layers of the positive electrode, the diaphragm and the negative electrode is arbitrary and is not particularly limited.
【００１１】[0011]
【作用】この発明に係る二次電池によれば、積層セルの
厚みを一定に保持することにより、サイクル数の増大に
伴う負極リチウムの脱落をさらに抑制することができ
る。積層セルの厚みを一定に保持することによるリチウ
ム脱落抑制の作用機構は明らかではないが、セルの厚み
が一定に保持される際、負極に圧力がかかることで、粒
状または針状に析出した負極リチウムまたはリチウム合
金の脱落が防止されると考えられた。According to the secondary battery of the present invention, by keeping the thickness of the laminated cell constant, it is possible to further suppress the loss of the negative electrode lithium due to the increase in the number of cycles. The mechanism of action of suppressing lithium loss by keeping the thickness of the laminated cell constant is not clear, but when the thickness of the cell is kept constant, pressure is applied to the negative electrode, so that the negative electrode deposited in a granular or acicular shape. It was thought that the loss of lithium or lithium alloy was prevented.
【００１２】[0012]
実施例１ １５ｍｍ×２５ｍｍサイズ（電極有効面積；端子取出し
部分を除く）の１００メッシュステンレス基板を準備
し、これの両面にポリアニリン膜を電解重合により形成
したものを正極として用いた。一方、端子取出し部分を
有する１５ｍｍ×２５ｍｍサイズ（電極有効面積）の１
００メッシュステンレス基板の両面に、厚さ０．２ｍｍ
のリチウム箔を圧着したものを負極として用いた。図１
に示すように、負極１／隔膜２／正極３／隔膜２／負極
１（電極３枚で２セル）の構成を有する積層セルスタッ
ク１０を形成し、両端の負極１、１にそれぞれ厚み５ｍ
ｍの四フッ化エチレン樹脂板４、４をあてがって四隅を
ビス−ナット５により止め、積層セルスタック１０を締
付けた。これにより、電極間距離が固定された。以上の
ように組立てを行なった積層セルスタックを電池容器に
組入れ、電解液を注入した。電解液として、１モル／ｌ
となるよう硼フッ化リチウムをプロピレンカーボネイト
に溶解したものを使用した。Example 1 A 100-mesh stainless steel substrate having a size of 15 mm × 25 mm (effective electrode area; excluding the terminal lead-out portion) was prepared, and a polyaniline film formed by electrolytic polymerization on both surfaces thereof was used as a positive electrode. On the other hand, 1 with a size of 15 mm × 25 mm (electrode effective area) that has a terminal lead-out portion
0.2 mm thick on both sides of 00 mesh stainless steel substrate
The one obtained by pressure-bonding the lithium foil of was used as a negative electrode. Figure 1
As shown in FIG. 5, a laminated cell stack 10 having a structure of negative electrode 1 / separation film 2 / positive electrode 3 / separation film 2 / negative electrode 1 (2 cells with 3 electrodes) is formed.
m tetrafluoroethylene resin plates 4 and 4 were applied, the four corners were fixed with screw-nuts 5, and the laminated cell stack 10 was tightened. This fixed the distance between the electrodes. The laminated cell stack assembled as described above was assembled in a battery container, and an electrolytic solution was injected. 1 mol / l as electrolyte
A solution of lithium borofluoride dissolved in propylene carbonate was used.
【００１３】以上のように構成される積層型リチウム系
二次電池において、正極３、負極１の端子取出し部分か
ら導線を引出し、充放電電流密度１ｍＡ／ｃｍ2 （７．
５ｍＡ；電流）、充電時間３０分の条件下、電圧２．７
Ｖまで放電した時点で充電に切換える充放電サイクル評
価を行なった。寿命の判定は、充電の終了が４．１Ｖと
なり、３０分の充電が不可能となった時点とした。な
お、電池評価はＡｒ置換雰囲気のドライボックス中で行
った。In the laminated lithium secondary battery constructed as described above, a lead wire is drawn out from the lead-out portions of the positive electrode 3 and the negative electrode 1, and the charge / discharge current density is 1 mA / cm 2 (7.
5 mA; current), charging time 30 minutes, voltage 2.7
A charge / discharge cycle evaluation was performed in which the charging was switched to charging at the time of discharging to V. The life was determined at the time when charging was terminated at 4.1 V and 30 minutes of charging became impossible. The battery was evaluated in a dry box in an Ar substitution atmosphere.
【００１４】実施例２ １００メッシュステンレス板にリチウム−アルミニウム
合金箔（アルミニウム２０重量％、厚み０．２ｍｍ）を
圧着したものを負極として用いたほかは、実施例１と同
様にして二次電池を構成し、同様の評価を行なった。Example 2 A secondary battery was prepared in the same manner as in Example 1 except that a 100-mesh stainless steel plate to which a lithium-aluminum alloy foil (aluminum 20% by weight, thickness 0.2 mm) was pressure bonded was used as the negative electrode. It was constructed and evaluated in the same manner.
【００１５】実施例３ 実施例１と同じ電極を図２に示すように、負極１／隔膜
２／正極３／隔膜２／負極１／隔膜２／正極３／隔膜２
／負極１／隔膜２／正極３／隔膜２／負極１／隔膜２／
正極３／隔膜２／負極１（電極８枚で８セル）の構成で
積層して積層セルスタック２０を形成した。これについ
て実施例１と同様に厚み５ｍｍの四フッ化エチレン樹脂
板２４、２４およびビス−ナット２５により締付けを行
なって、積層セルスタック２０の電極間距離を固定し
た。以上のように構成される積層型リチウム系二次電池
において、正極３、負極１の端子取出し部分から導線を
引出し、正極３、負極１につながる導線同士をそれぞれ
圧着端子で固定し、通電を行ない、実施例１と同様に評
価を行なった。Example 3 As shown in FIG. 2, the same electrode as in Example 1 was used, as shown in FIG. 2, negative electrode 1 / separation film 2 / positive electrode 3 / separation film 2 / negative electrode 1 / separation film 2 / positive electrode 3 / separation film 2
/ Negative electrode 1 / Differential membrane 2 / Positive electrode 3 / Differential membrane 2 / Negative electrode 1 / Differential membrane 2 /
A laminated cell stack 20 was formed by laminating in the configuration of positive electrode 3 / separation film 2 / negative electrode 1 (8 cells with 8 cells). Similar to Example 1, this was tightened with 5 mm thick tetrafluoroethylene resin plates 24, 24 and a screw-nut 25 to fix the distance between the electrodes of the laminated cell stack 20. In the laminated lithium-based secondary battery configured as described above, lead wires are drawn from the terminal lead-out portions of the positive electrode 3 and the negative electrode 1, and the lead wires connected to the positive electrode 3 and the negative electrode 1 are fixed with crimp terminals to conduct electricity. The evaluation was performed in the same manner as in Example 1.
【００１６】実施例４ １００メッシュステンレス板に上記リチウム−アルミニ
ウム合金箔を圧着したものを負極として用いたほかは、
実施例３と同様にして二次電池を形成し、同様に評価を
行なった。Example 4 In addition to using as a negative electrode, a 100 mesh stainless steel plate to which the above lithium-aluminum alloy foil was pressure bonded was used.
A secondary battery was formed in the same manner as in Example 3 and evaluated in the same manner.
【００１７】比較例１ 積層セルの締付けをテフロンテープを巻き付けることに
よって行なったほかは、実施例１と同様にして二次電池
を形成し、評価を行なった。Comparative Example 1 A secondary battery was formed and evaluated in the same manner as in Example 1 except that the laminated cell was tightened by winding a Teflon tape.
【００１８】比較例２ 積層セルの締付けをテフロンテープを巻き付けることに
よって行なったほかは、実施例２と同様にして二次電池
を形成し、評価を行なった。Comparative Example 2 A secondary battery was formed and evaluated in the same manner as in Example 2 except that the laminated cell was tightened by winding a Teflon tape.
【００１９】比較例３ 積層セルの締付けをテフロンテープを巻き付けることに
よって行なったほかは、実施例３と同様にして二次電池
を形成し、評価を行なった。Comparative Example 3 A secondary battery was formed and evaluated in the same manner as in Example 3, except that the laminated cell was tightened by winding a Teflon tape.
【００２０】比較例４ 積層セルの締付けをテフロンテープを巻き付けることに
よって行なったほかは、実施例４と同様にして二次電池
を形成し、評価を行なった。Comparative Example 4 A secondary battery was formed and evaluated in the same manner as in Example 4, except that the laminated cell was fastened by winding a Teflon tape.
【００２１】以上の実施例１〜４、比較例１〜４につい
て、充放電サイクル評価の結果を表１に示す。Table 1 shows the results of charge / discharge cycle evaluation for the above Examples 1 to 4 and Comparative Examples 1 to 4.
【００２２】[0022]
【表１】 セルの厚みが固定されるビスの締付けと、その厚みが変
動するテフロンテープでの締付けとを比較することによ
り、積層セルの厚みを固定して一定に保持することによ
り、サイクル寿命が向上することが明らかとなった。[Table 1] By comparing the tightening of screws with fixed cell thickness and the tightening with Teflon tape with varying thickness, the cycle life can be improved by keeping the laminated cell thickness fixed and constant. Became clear.
【００２３】なお、上記具体例では、押さえ板およびビ
スにより積層セルを固定しているが、固定手段はこれに
限定されず、積層セルスタックの厚みを一定に保つこと
ができれば、どのような手段を用いてもよい。In the above specific example, the laminated cell is fixed by the pressing plate and the screw, but the fixing means is not limited to this, and any means can be used if the thickness of the laminated cell stack can be kept constant. May be used.
【００２４】[0024]
【発明の効果】以上説明したとおり、この発明の係る積
層型リチウム系二次電池では、並列積層セル間の距離を
一定にすることにより、粒状または針状に析出し膨脹し
た負極リチウムまたはリチウム合金に圧力をかけ、その
脱落を防止する。その結果、負極の容量低下を防止する
ことができ、電池の寿命を伸ばすことが可能になる。し
たがって、この発明はサイクル特性の優れた積層型リチ
ウム系二次電池を提供する。As described above, in the laminated lithium secondary battery according to the present invention, by keeping the distance between the parallel laminated cells constant, the negative electrode lithium or lithium alloy that is expanded in the form of particles or needles is expanded. Apply pressure to prevent it from falling off. As a result, it is possible to prevent the capacity of the negative electrode from decreasing, and it is possible to extend the life of the battery. Therefore, the present invention provides a laminated lithium secondary battery having excellent cycle characteristics.
【図１】この発明に従う積層型リチウム系二次電池の１
具体例を示す斜視図である。FIG. 1 is a stack type lithium secondary battery 1 according to the present invention.
It is a perspective view which shows a specific example.
【図２】この発明に従う積層型リチウム系二次電池の他
の具体例を示す模式図である。FIG. 2 is a schematic view showing another specific example of the laminated lithium secondary battery according to the present invention.
１ 負極 ２ 隔膜 ３ 正極 ４ 四フッ化エチレン樹脂板 ５ ビス 1 negative electrode 2 diaphragm 3 positive electrode 4 tetrafluoroethylene resin plate 5 screw
Claims (2)
層セルを有する積層型リチウム系二次電池において、 前記積層セルにおいて電極を積層した方向の厚みが一定
に保持される、積層型リチウム系二次電池。1. A laminated lithium secondary battery having a laminated cell in which a positive electrode and a negative electrode are stacked with a diaphragm interposed therebetween, wherein the thickness of the laminated cell in the direction in which the electrodes are stacked is kept constant. Lithium secondary battery.
よびカーボンリチウム層間化合物の少なくともいずれか
である、請求項１の積層型リチウム系二次電池。2. The stacked lithium secondary battery according to claim 1, wherein the negative electrode is at least one of lithium, a lithium alloy and a carbon lithium intercalation compound.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP4088812A JPH05290886A (en) | 1992-04-09 | 1992-04-09 | Layered type lithium secondary battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP4088812A JPH05290886A (en) | 1992-04-09 | 1992-04-09 | Layered type lithium secondary battery |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH05290886A true JPH05290886A (en) | 1993-11-05 |
Family
ID=13953315
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP4088812A Withdrawn JPH05290886A (en) | 1992-04-09 | 1992-04-09 | Layered type lithium secondary battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH05290886A (en) |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001093577A (en) * | 1999-09-20 | 2001-04-06 | Toyota Central Res & Dev Lab Inc | Lithium secondary battery |
| JP2006252831A (en) * | 2005-03-09 | 2006-09-21 | Toyota Motor Corp | Manufacturing method of secondary battery, limitation tool of secondary battery, charging/discharging device and charging device of secondary battery |
| WO2007072713A1 (en) * | 2005-12-22 | 2007-06-28 | Fuji Jukogyo Kabushiki Kaisha | Lithium metal foil for battery or capacitor |
-
1992
- 1992-04-09 JP JP4088812A patent/JPH05290886A/en not_active Withdrawn
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001093577A (en) * | 1999-09-20 | 2001-04-06 | Toyota Central Res & Dev Lab Inc | Lithium secondary battery |
| JP2006252831A (en) * | 2005-03-09 | 2006-09-21 | Toyota Motor Corp | Manufacturing method of secondary battery, limitation tool of secondary battery, charging/discharging device and charging device of secondary battery |
| WO2007072713A1 (en) * | 2005-12-22 | 2007-06-28 | Fuji Jukogyo Kabushiki Kaisha | Lithium metal foil for battery or capacitor |
| US8685117B2 (en) | 2005-12-22 | 2014-04-01 | Fuji Jukogyo Kabushiki Kaisha | Lithium metal foil for battery or capacitor |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| A300 | Application deemed to be withdrawn because no request for examination was validly filed |
Free format text: JAPANESE INTERMEDIATE CODE: A300 Effective date: 19990706 |