JPH11214041A - Lithium ion secondary battery and manufacture thereof - Google Patents
Lithium ion secondary battery and manufacture thereofInfo
- Publication number
- JPH11214041A JPH11214041A JP10014472A JP1447298A JPH11214041A JP H11214041 A JPH11214041 A JP H11214041A JP 10014472 A JP10014472 A JP 10014472A JP 1447298 A JP1447298 A JP 1447298A JP H11214041 A JPH11214041 A JP H11214041A
- Authority
- JP
- Japan
- Prior art keywords
- separator
- lithium ion
- secondary battery
- ion secondary
- electrolyte
- 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.)
- Granted
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
- Cell Separators (AREA)
- Secondary Cells (AREA)
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、充放電サイクル寿
命が向上されたリチウムイオン２次電池及びその製造方
法に関する。The present invention relates to a lithium ion secondary battery having an improved charge / discharge cycle life and a method for manufacturing the same.
【０００２】[0002]
【従来の技術】従来より、各種用途にリチウムイオン２
次電池を使用するために、そのサイクル寿命を向上させ
ることが要望されている。例えば、特開平４−１１２４
６０号公報には、正極と負極との間に電解質を含浸させ
たゲル状電解質を介在させることにより、デンドライト
の析出を防止し、サイクル寿命を向上させる技術が開示
されている。2. Description of the Related Art Conventionally, lithium ion 2
In order to use a secondary battery, it is required to improve the cycle life. For example, Japanese Unexamined Patent Publication No.
No. 60 discloses a technique of interposing a gel electrolyte impregnated with an electrolyte between a positive electrode and a negative electrode, thereby preventing dendrite precipitation and improving cycle life.
【０００３】また、特開平９−２２７２６号公報には、
マイクロポーラスなポリオレフィンシートの両面に、電
解質を保持したポリマーが配された構造が開示されてい
る。これによれば、誤使用の際にポリオレフィンの融解
によりリチウムイオンの透過が妨げられ、電池機能を停
止するので、安全性が確保されるとされている。[0003] Also, Japanese Patent Application Laid-Open No. 9-22726 discloses that
A structure in which a polymer holding an electrolyte is disposed on both sides of a microporous polyolefin sheet is disclosed. According to this, the melting of the polyolefin hinders the permeation of lithium ions at the time of misuse and stops the battery function, so that safety is ensured.
【０００４】[0004]
【発明が解決しようとする課題】しかし、上記従来技術
のうち、正極と負極との間に電解質を含浸させたゲル状
電解質を介在させたものでは、高温でこのゲル状電解質
が流動化し、正極、負極が短絡してしまうという問題が
あった。However, among the above-mentioned prior arts, when a gel electrolyte impregnated with an electrolyte is interposed between a positive electrode and a negative electrode, the gel electrolyte fluidizes at a high temperature, and In addition, there is a problem that the negative electrode is short-circuited.
【０００５】また、マイクロポーラスなポリオレフィン
シートを使用する場合、ポリオレフィンのポーラス部で
デンドライトの生成の可能性があり、正極、負極が短絡
してしまうという問題があった。Further, when a microporous polyolefin sheet is used, there is a possibility that dendrites may be generated in the porous portion of the polyolefin, and there is a problem that the positive electrode and the negative electrode are short-circuited.
【０００６】従って、いずれの場合にもサイクル寿命を
十分向上させることができなかった。Therefore, in any case, the cycle life could not be sufficiently improved.
【０００７】本発明は、上記従来の課題に鑑みなされた
ものであり、その目的は、充放電サイクル寿命が向上さ
れたリチウムイオン２次電池及びその製造方法を提供す
ることにある。The present invention has been made in view of the above-mentioned conventional problems, and has as its object to provide a lithium ion secondary battery having an improved charge / discharge cycle life and a method for manufacturing the same.
【０００８】[0008]
【課題を解決するための手段】上記目的を達成するため
に、本発明は、リチウムイオン２次電池であって、融点
２００℃以下のポリオレフィンと電解質を保持したポリ
マーとが均一に分散しているセパレータを有することを
特徴とする。In order to achieve the above object, the present invention relates to a lithium ion secondary battery in which a polyolefin having a melting point of 200 ° C. or less and a polymer holding an electrolyte are uniformly dispersed. It has a separator.
【０００９】また、上記リチウムイオン２次電池の製造
方法であって、粒径が１００μｍ以下で融点が２００℃
以下のポリオレフィン粒子と電解質を保持するポリマー
粒子とを均一に混合する工程と、この混合物を用いて１
０〜１００μｍの厚さのシートを形成する工程と、この
シートに電解液を含浸する工程と、を有することを特徴
とする。Further, in the method for producing a lithium ion secondary battery, the particle size is 100 μm or less and the melting point is 200 ° C.
A step of uniformly mixing the following polyolefin particles and polymer particles holding an electrolyte, and 1
It has a step of forming a sheet having a thickness of 0 to 100 μm and a step of impregnating the sheet with an electrolytic solution.
【００１０】[0010]
【発明の実施の形態】以下、本発明の実施の形態（以下
実施形態という）を、図面に従って説明する。Embodiments of the present invention (hereinafter referred to as embodiments) will be described below with reference to the drawings.
【００１１】図１には、本発明に係るリチウムイオン２
次電池に使用されるセパレータの例が示される。図１に
おいて、セパレータは、ポリエチレン（ＰＥ）又はポリ
プロピレン（ＰＰ）のようなポリオレフィン粒子１０
が、ＰＶＤＦ−ＨＦＰやＰＡＮ等、電解液を含有して膨
潤する性質を有するポリマー粒子１２とともに均一に混
合された構造となっている。FIG. 1 shows a lithium ion 2 according to the present invention.
An example of a separator used for a secondary battery is shown. In FIG. 1, a separator is made of polyolefin particles 10 such as polyethylene (PE) or polypropylene (PP).
Has a structure in which it is uniformly mixed with polymer particles 12 such as PVDF-HFP and PAN which have the property of swelling by containing an electrolytic solution.
【００１２】ポリオレフィン粒子１０は、１００μｍ以
下の粒径を有している。材質としては、融点が２００℃
以下であることが望ましく、例えば上述のＰＥあるいは
ＰＰの粒子が好適である。なお、ポリオレフィン粒子１
０は、図に示されるような粒子状に限らず、繊維状とす
ることも可能である。The polyolefin particles 10 have a particle size of 100 μm or less. The material has a melting point of 200 ° C
It is desirable that the particle size is as follows, for example, the above-mentioned PE or PP particles are preferable. The polyolefin particles 1
0 is not limited to a particle shape as shown in the figure, but may be a fibrous shape.
【００１３】また、ポリマー粒子１２としては、ＰＶＤ
Ｆ−ＨＦＰ等が使用される。これらは、電解液を含浸さ
せると膨潤する樹脂である。The polymer particles 12 are PVD.
F-HFP or the like is used. These are resins that swell when impregnated with an electrolytic solution.
【００１４】これらのポリオレフィン粒子１０及びポリ
マー粒子１２を混合し、１０〜１００μｍの厚みのシー
トを形成し、セパレータとする。なお、ポリオレフィン
粒子１０と、ポリマー粒子１２との混合割合は、ポリマ
ー粒子１２中に電解液を含浸させた状態で、ポリオレフ
ィン粒子：ポリマー粒子（含電解液）＝２：８〜７：３
が好適である。このようなセパレータは、まずポリオレ
フィン粒子１０とポリマー粒子１２とを均一に混合し、
この混合物から上記厚さのシートを作製し、これに電解
液を含浸することによって製造する。The polyolefin particles 10 and the polymer particles 12 are mixed to form a sheet having a thickness of 10 to 100 μm, which is used as a separator. The mixing ratio of the polyolefin particles 10 and the polymer particles 12 is such that polyolefin particles: polymer particles (electrolyte-containing solution) = 2: 8 to 7: 3 in a state where the polymer particles 12 are impregnated with the electrolytic solution.
Is preferred. Such a separator first mixes the polyolefin particles 10 and the polymer particles 12 uniformly,
A sheet having the above thickness is prepared from this mixture, and the sheet is impregnated with an electrolytic solution to produce the sheet.
【００１５】以上のようにして構成した本発明に係るリ
チウムイオン２次電池のセパレータは、高電流で充放電
を実施しても、デンドライトの生成がなく、これによる
短絡を防止することができる。これは以下の理由による
ものと考えられる。[0015] The separator of the lithium ion secondary battery according to the present invention configured as described above does not generate dendrites even when charging and discharging are performed at a high current, so that a short circuit due to the dendrites can be prevented. This is considered to be due to the following reasons.
【００１６】従来のセパレータは、図２に示されるよう
に、基材１４に多数の細孔１６が設けられている。リチ
ウムイオンはこの細孔１６を通過していく。しかし、図
２に示される従来のセパレータでは、リチウムイオンは
基材１４に一定密度で設けられた細孔１６のみを通過し
ていく。従って、セパレータの両面側の電位差は、この
細孔１６の部分で生じることになる。すなわち、リチウ
ムイオン２次電池に大きな充放電電流を流した場合に
は、この細孔１６の部分のみでリチウムイオンが移動
し、この部分に局所的に大きな電流が流れる。このた
め、リチウムイオンが通過する細孔１６の出口側での電
位が局所的に大きく低下し、リチウム電位まで低下する
可能性がある。ここの電位がリチウム電位まで低下する
と、リチウムイオンは金属リチウムとなり、これが発達
してデンドライトとなる。このデンドライトによりリチ
ウムイオン２次電池内部でセパレータの短絡が生じる。In the conventional separator, as shown in FIG. 2, a large number of pores 16 are provided in a substrate 14. Lithium ions pass through the pores 16. However, in the conventional separator shown in FIG. 2, lithium ions pass only through the pores 16 provided at a constant density on the substrate 14. Therefore, a potential difference between both sides of the separator is generated in the portion of the pores 16. That is, when a large charging / discharging current is applied to the lithium ion secondary battery, lithium ions move only in the portion of the pore 16, and a large current flows locally in this portion. For this reason, the potential on the exit side of the pore 16 through which the lithium ions pass may be significantly reduced locally, and may decrease to the lithium potential. When the potential here drops to the lithium potential, lithium ions become metallic lithium, which develops into dendrites. This dendrite causes a short circuit of the separator inside the lithium ion secondary battery.
【００１７】これに対して、図１に示された本発明に係
るセパレータでは、ポリオレフィン粒子１０の間すなわ
ちポリマー粒子１２が充填された部分を、比較的自由に
リチウムイオンが移動することができる。しかもこの移
動方向は、図２に示された例に比べ様々な方向が可能で
ある。従って、大きな充放電電流を流した場合にも、局
所的に大きな電流が流れることを防止できる。すなわ
ち、本発明においては、図２に示された細孔１６を、セ
パレータ全体に均一に分散したことになり、このため、
セパレータ中の電流密度の均一化を図ることができ、局
所的に大きな電流が流れることを防止することができて
いる。このため、リチウムイオンが移動する際のセパレ
ータの下流側で、電位がリチウム電位まで低下すること
がなく、デンドライトの発生を防止することができてい
る。On the other hand, in the separator according to the present invention shown in FIG. 1, lithium ions can relatively freely move between the polyolefin particles 10, that is, the portion filled with the polymer particles 12. In addition, this moving direction can be various directions as compared with the example shown in FIG. Therefore, even when a large charge / discharge current flows, it is possible to prevent a large current from flowing locally. That is, in the present invention, the pores 16 shown in FIG. 2 are uniformly dispersed throughout the separator.
The current density in the separator can be made uniform, and a large current can be prevented from flowing locally. For this reason, the potential does not decrease to the lithium potential downstream of the separator when the lithium ions move, so that the generation of dendrites can be prevented.
【００１８】また、図１に示されたセパレータでは、ポ
リオレフィン粒子１０として、融点が２００℃以下のＰ
ＥやＰＰが使用されているので、仮に、リチウムイオン
２次電池内に局所的な電流密度の上昇が生じ、局所的に
温度が上昇した場合でも、これらのポリオレフィン粒子
１０が溶融し、セパレータの目を詰める。この結果、そ
の部分でのリチウムイオンの移動を停止する。これによ
り、局所的な電流密度の上昇を抑制でき、シャットダウ
ン機能を発揮する。In the separator shown in FIG. 1, the polyolefin particles 10 have a melting point of 200 ° C. or less.
Since E or PP is used, even if the current density locally increases in the lithium ion secondary battery and the temperature locally increases, these polyolefin particles 10 are melted and the separator Close your eyes. As a result, the movement of lithium ions in that portion is stopped. Thereby, a local increase in the current density can be suppressed, and the shutdown function is exhibited.
【００１９】以下、本発明に係るリチウムイオン２次電
池のセパレータの具体例を実施例として説明する。Hereinafter, specific examples of the separator of the lithium ion secondary battery according to the present invention will be described as examples.
【００２０】実施例．平均粒径１０μｍのＰＥ８．５ｇ
とＰＶＤＦ−ＨＦＰ１．５ｇとＴＨＦ２０ｇとを５０℃
で１時間混合し、その後室温まで冷却した。次に、ドク
ターブレード法により薄膜を形成し、８０℃で乾燥させ
た。これにより３０μｍの厚さのセパレータを得た。Embodiment 1 8.5 g of PE having an average particle size of 10 μm
And 1.5 g of PVDF-HFP and 20 g of THF at 50 ° C.
For 1 hour and then cooled to room temperature. Next, a thin film was formed by a doctor blade method and dried at 80 ° C. Thus, a separator having a thickness of 30 μm was obtained.
【００２１】正極としてＬｉＭｎ2Ｏ4、負極として金属
リチウムを使用し、上述のセパレータを介して対向配置
させた。これを、１ｍｏｌＬｉＢＦ4−ＥＣ：ＤＥＣ＝
１：１の電解液に浸漬してリチウムイオン２次電池を作
製した。なお、上記正極は、ＬｉＭｎ2Ｏ4にカーボンブ
ラックを１０％添加し、Ｎ−メチルピロリドン（ＮＭ
Ｐ）中で１０分攪拌して正極ペーストとし、この正極ペ
ーストから形成したものである。この正極は、カーボン
ブラックが十分分散されていないため、平均１００μ
ｍ、最大３００μｍの凹凸が存在した。この凹凸を有す
る正極を用いて充電電流を増加させ、電気特性を調べ
た。LiMn 2 O 4 was used as a positive electrode, and metallic lithium was used as a negative electrode. This was converted to 1 mol LiBF 4 -EC: DEC =
The battery was immersed in a 1: 1 electrolyte to prepare a lithium ion secondary battery. The positive electrode was prepared by adding 10% of carbon black to LiMn 2 O 4 and adding N-methylpyrrolidone (NM
The mixture was stirred in P) for 10 minutes to form a positive electrode paste, and was formed from this positive electrode paste. This positive electrode has an average of 100 μm because carbon black is not sufficiently dispersed.
m, irregularities of up to 300 μm were present. The charging current was increased using the positive electrode having the irregularities, and the electrical characteristics were examined.
【００２２】なお、比較例として、従来のＰＥ性の多孔
質膜とＰＶＤＦ−ＨＦＰを電解液で膨潤させたポリマー
粒子のみから構成したセパレータとをあわせて評価し
た。As a comparative example, a conventional PE porous film and a separator composed only of polymer particles obtained by swelling PVDF-HFP with an electrolytic solution were evaluated.
【００２３】充電電流を増加させていった場合、ＰＥの
多孔質膜で形成されたセルの場合には、５Ｃの電流値で
短絡が発生した。また、ＰＶＤＦ−ＨＦＰを電解液で膨
潤させたセパレータでは８Ｃの電流値で短絡が発生し
た。これに対して、上述した本発明に係るセパレータで
は、２０Ｃの電流値でも短絡は発生しなかった。When the charging current was increased, a short circuit occurred at a current value of 5 C in the case of a cell formed of a porous film of PE. Further, in the separator in which PVDF-HFP was swollen with the electrolytic solution, a short circuit occurred at a current value of 8C. On the other hand, in the separator according to the present invention described above, no short circuit occurred even at a current value of 20C.
【００２４】ＰＶＤＦ−ＨＦＰを電解液で膨潤させたセ
パレータでは、もともとリチウムイオンを通過させるの
で、シャットダウン機能がないうえ、局所的な電流密度
の上昇により温度が高くなると、ゲルの流動化により、
電極同士の短絡が発生する。このため、本発明に比べて
小さな電流で短絡が発生するものと考えられる。In a separator in which PVDF-HFP is swollen with an electrolytic solution, lithium ions are originally allowed to pass therethrough, so there is no shutdown function, and when the temperature rises due to a local increase in current density, the gel becomes fluidized due to fluidization.
A short circuit between the electrodes occurs. Therefore, it is considered that a short circuit occurs with a smaller current than in the present invention.
【００２５】[0025]
【発明の効果】以上説明したように、本発明によれば、
ポリオレフィン粒子とポリマー粒子とを均一に混合し、
電流密度の均一化を図っているので、局所的な高電流を
防止でき、デンドライトの発生を抑制することができ
る。この結果、充放電サイクル寿命を向上させることが
できた。As described above, according to the present invention,
Mixing polyolefin particles and polymer particles uniformly,
Since the current density is made uniform, local high current can be prevented, and generation of dendrite can be suppressed. As a result, the charge / discharge cycle life was able to be improved.
【００２６】また、局所的に電流密度が上昇した場合に
も、温度の上昇により、ポリオレフィン粒子が溶融し、
リチウムイオンの通過を抑制するシャットダウン機能を
有するので、局所的な大電流による故障を防止すること
ができる。Further, even when the current density locally increases, the polyolefin particles are melted by the increase in temperature,
Since it has a shutdown function for suppressing passage of lithium ions, it is possible to prevent a failure due to a local large current.
【図１】 本発明に係るリチウムイオン２次電池に使用
されるセパレータを示す図である。FIG. 1 is a view showing a separator used in a lithium ion secondary battery according to the present invention.
【図２】 従来における細孔を有するセパレータを示す
図である。FIG. 2 is a view showing a conventional separator having pores.
１０ ポリオレフィン粒子、１２ ポリマー粒子、１４
基材、１６ 細孔。10 polyolefin particles, 12 polymer particles, 14
Substrate, 16 pores.
Claims (2)
解質を保持したポリマーとが均一に分散しているセパレ
ータを有することを特徴とするリチウムイオン２次電
池。1. A lithium ion secondary battery comprising a separator in which a polyolefin having a melting point of 200 ° C. or lower and a polymer holding an electrolyte are uniformly dispersed.
以下のポリオレフィン粒子と電解質を保持するポリマー
粒子とを均一に混合する工程と、この混合物を用いて１
０〜１００μｍの厚さのシートを形成する工程と、前記
シートに電解液を含浸する工程と、を有することを特徴
とするリチウムイオン２次電池の製造方法。2. A particle size of 100 μm or less and a melting point of 200 ° C.
A step of uniformly mixing the following polyolefin particles and polymer particles holding an electrolyte, and 1
A method for producing a lithium ion secondary battery, comprising: a step of forming a sheet having a thickness of 0 to 100 μm; and a step of impregnating the sheet with an electrolytic solution.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP01447298A JP3994496B2 (en) | 1998-01-27 | 1998-01-27 | Lithium ion secondary battery and manufacturing method thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP01447298A JP3994496B2 (en) | 1998-01-27 | 1998-01-27 | Lithium ion secondary battery and manufacturing method thereof |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH11214041A true JPH11214041A (en) | 1999-08-06 |
| JP3994496B2 JP3994496B2 (en) | 2007-10-17 |
Family
ID=11862013
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP01447298A Expired - Fee Related JP3994496B2 (en) | 1998-01-27 | 1998-01-27 | Lithium ion secondary battery and manufacturing method thereof |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3994496B2 (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001243988A (en) * | 2000-02-28 | 2001-09-07 | Nitto Denko Corp | Film shape electrolyte |
| JP2006173001A (en) * | 2004-12-17 | 2006-06-29 | Nissan Motor Co Ltd | Lithium-ion battery and its manufacturing method |
| CN105680086A (en) * | 2014-12-03 | 2016-06-15 | 纳米及先进材料研发院有限公司 | Lithium ion battery with thermal sensitive layer |
| JP2016162487A (en) * | 2015-02-26 | 2016-09-05 | トヨタ自動車株式会社 | Method of manufacturing secondary battery |
-
1998
- 1998-01-27 JP JP01447298A patent/JP3994496B2/en not_active Expired - Fee Related
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2001243988A (en) * | 2000-02-28 | 2001-09-07 | Nitto Denko Corp | Film shape electrolyte |
| JP4601114B2 (en) * | 2000-02-28 | 2010-12-22 | 日東電工株式会社 | Thin film electrolyte |
| JP2006173001A (en) * | 2004-12-17 | 2006-06-29 | Nissan Motor Co Ltd | Lithium-ion battery and its manufacturing method |
| JP4734912B2 (en) * | 2004-12-17 | 2011-07-27 | 日産自動車株式会社 | Lithium ion battery and manufacturing method thereof |
| CN105680086A (en) * | 2014-12-03 | 2016-06-15 | 纳米及先进材料研发院有限公司 | Lithium ion battery with thermal sensitive layer |
| JP2016162487A (en) * | 2015-02-26 | 2016-09-05 | トヨタ自動車株式会社 | Method of manufacturing secondary battery |
Also Published As
| Publication number | Publication date |
|---|---|
| JP3994496B2 (en) | 2007-10-17 |
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