JPH07220759A - Nonaqueous electrolyte secondary battery - Google Patents
Nonaqueous electrolyte secondary batteryInfo
- Publication number
- JPH07220759A JPH07220759A JP6010091A JP1009194A JPH07220759A JP H07220759 A JPH07220759 A JP H07220759A JP 6010091 A JP6010091 A JP 6010091A JP 1009194 A JP1009194 A JP 1009194A JP H07220759 A JPH07220759 A JP H07220759A
- Authority
- JP
- Japan
- Prior art keywords
- active material
- electrode
- negative electrode
- protective film
- material layer
- 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
- Battery Electrode And Active Subsutance (AREA)
- Secondary Cells (AREA)
Abstract
Description
【０００１】[0001]
【産業上の利用分野】本発明は、例えば負極活物質とし
て炭素材料のようなリチウムイオンをドープ・脱ドープ
することが可能な物質を用い、正極活物質としてリチウ
ムコバルト複合酸化物等のリチウム複合酸化物を用いる
非水電解液二次電池に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention uses, for example, a material such as a carbon material that can be doped with lithium ions and dedoped, as a negative electrode active material, and a lithium complex such as a lithium cobalt complex oxide as a positive electrode active material. The present invention relates to a non-aqueous electrolyte secondary battery using an oxide.
【０００２】[0002]
【従来の技術】近年、電子技術の進歩により、電子機器
の高性能化，小型化，ポータブル化が進み、これら電子
機器に使用される電池に対しても高いエネルギー密度を
有することが強く要求されるようになっている。2. Description of the Related Art In recent years, due to advances in electronic technology, high performance, miniaturization, and portability of electronic devices have been advanced, and batteries used in these electronic devices are also strongly required to have high energy density. It has become so.
【０００３】従来、これら電子機器に使用される二次電
池としては、ニッケル・カドミウム電池や鉛電池等の水
系電解液二次電池が挙げられる、これら電池は、放電電
圧が低く、エネルギー密度の高い電池を得るという点で
は不十分である。Conventionally, secondary batteries used in these electronic devices include aqueous electrolyte secondary batteries such as nickel-cadmium batteries and lead batteries. These batteries have low discharge voltage and high energy density. It is insufficient in terms of obtaining a battery.
【０００４】そこで、最近、上述のニッケル・カドミウ
ム電池などに代わる二次電池として、負極活物質として
炭素材料のようなリチウムイオンをドープ・脱ドープす
ることが可能な物質を用い、正極活物質としてリチウム
コバルト複合酸化物等のリチウム複合酸化物を用い、電
解液として非水溶媒にリチウム塩を溶解してなる非水電
解液を用いる非水電解液二次電池の研究・開発が盛んに
行われている。Therefore, recently, as a secondary battery replacing the above-mentioned nickel-cadmium battery or the like, a material capable of doping / dedoping lithium ions such as a carbon material is used as a negative electrode active material and a positive electrode active material is used. Research and development of non-aqueous electrolyte secondary batteries using lithium composite oxides such as lithium cobalt composite oxides and non-aqueous electrolytes prepared by dissolving lithium salt in a non-aqueous solvent as electrolytes have been actively conducted. ing.
【０００５】この電池は、電池電圧が高く、自己放電も
少ないといった長所を有し、高いエネルギー密度を発揮
する。This battery has the advantages that the battery voltage is high and self-discharge is small, and exhibits a high energy density.
【０００６】上記炭素材料やリチウム複合酸化物を実際
に活物質として用いるには、これらを平均粒径５〜５０
μｍの粉末とし、バインダーとともに溶媒に分散させて
負極合剤スラリー，正極合剤スラリーをそれぞれ調製す
る。そして、この各スラリーを集電体となる金属箔に塗
布し、負極活物質層，正極活物質層を形成する。この集
電体に負極活物質層，正極活物質層がそれぞれ積層され
た形の負極，正極を、間にセパレータを介して互いを隔
離し、その状態で電池缶内に収納する。In order to actually use the above-mentioned carbon materials and lithium composite oxides as active materials, these are used with an average particle size of 5-50.
A powder having a diameter of μm is dispersed in a solvent together with a binder to prepare a negative electrode mixture slurry and a positive electrode mixture slurry. Then, each of the slurries is applied to a metal foil serving as a current collector to form a negative electrode active material layer and a positive electrode active material layer. A negative electrode and a positive electrode each having a negative electrode active material layer and a positive electrode active material layer laminated on this current collector are separated from each other with a separator interposed therebetween, and housed in the battery can in this state.
【０００７】ここで、上述のような非水電解液二次電池
において注意する点は、これに用いられる非水電解液
が、水系電解液に比べると電導度が２桁位小さいことで
ある。したがって、十分な電池性能を得るには、電池の
構造をできるだけ電解質が移動し易いかたちとすること
が必要となる。Here, a point to be noted in the above-mentioned non-aqueous electrolyte secondary battery is that the non-aqueous electrolyte used therein has an electric conductivity that is about two orders of magnitude smaller than that of the aqueous electrolyte. Therefore, in order to obtain sufficient battery performance, it is necessary to make the structure of the battery such that the electrolyte can move as easily as possible.
【０００８】このため、上記非水電解液二次電池では、
正極と負極を隔離するためのセパレータとして、厚さ１
０〜５０μｍ程度の非常に薄いセパレータを使用するよ
うにしている。Therefore, in the above non-aqueous electrolyte secondary battery,
As a separator to separate the positive and negative electrodes, thickness 1
A very thin separator of about 0 to 50 μm is used.
【０００９】[0009]
【発明が解決しようとする課題】ところで、上述の如く
非水電解液二次電池において、電極は集電体上に粉末の
活物質を含んだ合剤スラリーを塗布して活物質層を積層
することで作製され、その後電池缶内に収納される。By the way, in the non-aqueous electrolyte secondary battery as described above, the electrode is coated with the mixture slurry containing the powdered active material on the current collector to form the active material layer. It is produced by that, and then stored in a battery can.
【００１０】このとき、活物質層が形成された電極は、
電池缶内に収納されるまでの間には、電極とセパレータ
との積層工程や所定の電極形状に裁断する裁断工程等，
各種工程を通過する。通常、これら工程は、大量生産を
目的として電極を長尺状の電極原反として作製し、これ
を巻き出しロール，巻き取りロール，ガイドローラ等の
走行系を用いて走行させ、この間に順次連続して行う。At this time, the electrode on which the active material layer is formed is
Before being stored in the battery can, the process of stacking the electrode and the separator, the process of cutting into a predetermined electrode shape, etc.
Passes through various processes. Usually, in these processes, for the purpose of mass production, the electrode is manufactured as a long electrode raw material, which is run using a running system such as an unwinding roll, a winding roll, a guide roller, etc. Then do.
【００１１】しかし、この電極原反の走行に際しては、
活物質層がガイドローラ等と接触することによって該活
物質層から活物質が脱落し、脱落した活物質の一部が電
極の表面に再び付着するといった不都合が生じている。However, when the raw material of the electrode is traveling,
When the active material layer comes into contact with a guide roller or the like, the active material drops off from the active material layer, and a part of the dropped active material reattaches to the surface of the electrode.
【００１２】電極表面に再付着した脱落活物質は、粒径
が５〜５０μｍとセパレータの厚みと略同じ程度である
ため、組み立てられた電池内でセパレータを貫通し、内
部ショートを引き起こすという問題を誘発する。Since the drop-out active material redeposited on the electrode surface has a particle size of 5 to 50 μm, which is about the same as the thickness of the separator, there is a problem that it penetrates the separator in the assembled battery and causes an internal short circuit. Induce.
【００１３】そこで、本発明はこのような従来の実情に
鑑みて提案されたものであり、製造に際する電極からの
活物質の脱落を抑え、内部ショートの発生が防止できる
非水電解液二次電池を提供することを目的とする。Therefore, the present invention has been proposed in view of such a conventional situation, and it is possible to prevent the active material from falling off from the electrode during manufacturing and prevent the occurrence of internal short circuit. The purpose is to provide a secondary battery.
【００１４】[0014]
【課題を解決するための手段】上述の目的を達成するた
めに、本発明の非水電解液二次電池は、集電体に負極活
物質塗布層を積層してなる負極と、集電体に正極活物質
塗布層を積層してなる正極と、非水電解液を有する非水
電解液二次電池において、上記負極活物質塗布層，正極
活物質塗布層の少なくともいずれかの表面に厚さ０．１
〜２００μｍの多孔性保護膜が形成されていることを特
徴とするものである。In order to achieve the above-mentioned object, a non-aqueous electrolyte secondary battery of the present invention comprises a negative electrode formed by laminating a negative electrode active material coating layer on a current collector, and a current collector. In a non-aqueous electrolyte secondary battery having a positive electrode having a positive electrode active material coating layer laminated thereon and a non-aqueous electrolyte solution, a thickness is provided on at least one surface of the negative electrode active material coating layer and the positive electrode active material coating layer. 0.1
It is characterized in that a porous protective film having a thickness of up to 200 μm is formed.
【００１５】また、多孔性保護膜は、不織布であること
を特徴とするものである。さらに、多孔性保護膜は、樹
脂結着剤と固体粒子からなることを特徴とするものであ
る。Further, the porous protective film is characterized by being a non-woven fabric. Furthermore, the porous protective film is characterized by comprising a resin binder and solid particles.
【００１６】本発明が適用される非水電解液二次電池
は、集電体に負極活物質層を積層してなる負極と、集電
体に正極活物質層を積層してなる正極と、非水電解液を
有してなるものである。The non-aqueous electrolyte secondary battery to which the present invention is applied includes a negative electrode formed by stacking a negative electrode active material layer on a current collector, and a positive electrode formed by stacking a positive electrode active material layer on a current collector. It has a non-aqueous electrolyte.
【００１７】本発明では、このような非水電解液二次電
池の内部ショートの発生を抑えるために、上記正極，負
極の少なくともいずれかの活物質層表面に多孔性保護膜
を形成することとする。In the present invention, in order to suppress the occurrence of an internal short circuit in such a non-aqueous electrolyte secondary battery, a porous protective film is formed on the surface of at least one of the positive electrode and negative electrode active material layers. To do.
【００１８】すなわち、このような非水電解液二次電池
において、正極，負極は、それぞれ集電体上に粉末の活
物質を含んだ合剤スラリーを塗布して活物質層を積層す
ることで作製され、その後電池缶内に収納される。ここ
で、活物質層が形成された電極は、電池缶内に収納され
るまでの間に、さらにセパレータとの積層工程や裁断工
程等，各種工程を通過する。この作製から電池缶への収
納までの間に、活物質層の特に表面付近に存在する活物
質が脱落し、さらにこの脱落活物質の一部が電極に再付
着する場合がある。電極に再付着した活物質は完成した
電池内で内部ショートを引き起こす原因となる。That is, in such a non-aqueous electrolyte secondary battery, the positive electrode and the negative electrode are each formed by applying a mixture slurry containing a powdered active material onto a current collector to form an active material layer. It is manufactured and then stored in a battery can. Here, the electrode on which the active material layer is formed passes through various steps such as a step of stacking with a separator and a step of cutting until it is housed in the battery can. During the period from the preparation to the storage in the battery can, the active material existing particularly near the surface of the active material layer may drop off, and a part of the dropped active material may reattach to the electrode. The active material redeposited on the electrodes causes an internal short circuit in the completed battery.
【００１９】そこで、本発明では、このような脱落活物
質によって発生する内部ショートを抑えるために、正
極，負極の少なくともいずれかの活物質層表面に、多孔
性保護膜を形成し、活物質層からの活物質の脱落を防止
することとする。Therefore, in the present invention, in order to suppress an internal short circuit caused by such a dropout active material, a porous protective film is formed on the surface of the active material layer of at least one of the positive electrode and the negative electrode, and the active material layer is formed. The active material should be prevented from falling off.
【００２０】活物質層形成後、その表面に上記多孔性保
護膜を形成すると、活物質層表面に存在する活物質が保
護膜に強固に結合される。このような保護膜形成後であ
れば、電極が電池缶内に収納されるまでの間に、表面に
多少の接触があったとしても、表面の活物質が保護膜に
強固に結合されているので、活物質が電極から脱落する
といったことがない。したがって、脱落活物質の再付着
によって誘発される上記内部ショートが防止されること
になる。When the porous protective film is formed on the surface of the active material layer after formation, the active material existing on the surface of the active material layer is firmly bonded to the protective film. After such a protective film is formed, the active material on the surface is firmly bonded to the protective film even if there is some contact with the surface before the electrode is housed in the battery can. Therefore, the active material does not fall off the electrode. Therefore, the internal short circuit caused by the redeposition of the drop-off active material is prevented.
【００２１】ここで、保護膜として多孔性のものを用い
るのは、電極の本来の機能，すなわち電解液中の電解質
イオンとの電極反応を保護膜が妨げるのを防止するため
である。The reason why the protective film is porous is to prevent the protective film from interfering with the original function of the electrode, that is, the electrode reaction with the electrolyte ions in the electrolytic solution.
【００２２】なお、この多孔性保護膜の厚さは、０．１
〜２００μｍの範囲とする必要がある。多孔性保護膜の
厚さが０．１μｍ未満の場合には、保護効果が不足し、
活物質の脱落を十分防止することができない。また、多
孔性保護膜の厚さが２００μｍを越える場合には、当該
保護膜が電極の電解液中イオンとの反応を妨げ、電池性
能が劣化する。The thickness of this porous protective film is 0.1.
It is necessary to be in the range of up to 200 μm. When the thickness of the porous protective film is less than 0.1 μm, the protective effect is insufficient,
It is not possible to sufficiently prevent the active material from falling off. Further, when the thickness of the porous protective film exceeds 200 μm, the protective film hinders the reaction of the electrodes with the ions in the electrolytic solution, which deteriorates the battery performance.
【００２３】このような多孔性保護膜としては、不織布
や、微粒子を結着剤とともに溶媒に分散させた微粒子ス
ラリーを塗布することで形成されるコーティング膜が挙
げられる。Examples of such a porous protective film include a non-woven fabric and a coating film formed by applying a fine particle slurry in which fine particles are dispersed in a solvent together with a binder.
【００２４】不織布としては、膜形成時の温度に耐え、
電解液の非水溶媒に不溶な材質のものを選択することが
必要であり、さらに単位面積当たりの重量を活物質脱落
防止効果を損なわない範囲でできるだけ小さくできるも
のが望ましい。例えばマニラ麻等が使用できる。また、
マニラ麻のように絶縁性材質に限らず、電極反応の円滑
性を考慮して電子伝導性を有するものであっても良い。As a non-woven fabric, it withstands the temperature during film formation,
It is necessary to select a material that is insoluble in the non-aqueous solvent of the electrolytic solution, and it is desirable that the weight per unit area can be made as small as possible without impairing the effect of preventing the active material from falling off. For example, Manila hemp or the like can be used. Also,
The material is not limited to an insulating material such as Manila hemp, but may be one having electron conductivity in consideration of smoothness of electrode reaction.
【００２５】活物質層表面に不織布を保持させるには、
接着剤等を用いても良いが、このような特別な手段を用
いなくとも、図１に示すように、集電体２１両面に活物
質２２を含有するスラリーを塗布して活物質塗膜２３を
形成し、この活物質塗膜２３が濡れた状態にあるうち
に、塗膜２３上に直接不織布２４を載せ、乾燥させれば
良い。活物質塗膜２３の乾燥とともに不織布２４がその
表面に貼着され、表面に不織り布が貼り合わされたかた
ちで活物質層が形成される。To retain the nonwoven fabric on the surface of the active material layer,
Although an adhesive agent or the like may be used, the slurry containing the active material 22 is applied to both surfaces of the current collector 21 and the active material coating film 23 as shown in FIG. While the active material coating film 23 is wet, the nonwoven fabric 24 may be directly placed on the coating film 23 and dried. As the active material coating film 23 is dried, the non-woven fabric 24 is attached to the surface thereof, and an active material layer is formed in the form of a non-woven fabric being attached to the surface.
【００２６】一方、上記多孔性保護膜としては、上述の
如く不織布以外に微粒子スラリーを塗布することで形成
されるコーティング膜であっても良い。On the other hand, the porous protective film may be a coating film formed by applying a fine particle slurry other than the non-woven fabric as described above.
【００２７】すなわち、図２に示すように、活物質２５
を含有する電極活物質層２６表面に微粒子２７が結着剤
とともに溶剤に分散されてなる微粒子スラリー２８を塗
布すると、スラリー２８中の結着剤が固体微粒子２７同
士の接触界面あるいは固体微粒子２７と活物質層２６と
の接触界面近傍に集まる。これにより、この接触界面以
外の部分がいわば孔の空いた状態になり、このような孔
部を多数有する保護膜が形成される。That is, as shown in FIG.
When the fine particle slurry 28 in which the fine particles 27 are dispersed in a solvent together with the binder is applied to the surface of the electrode active material layer 26 containing, the binder in the slurry 28 forms a contact interface between the solid fine particles 27 or the solid fine particles 27. Collect near the contact interface with the active material layer 26. As a result, a portion other than the contact interface becomes, so to speak, a hole, and a protective film having many such hole portions is formed.
【００２８】上記微粒子スラリーに含有させる微粒子と
しては、電解液の非水溶媒に不溶であることが必要であ
り、アルミナ粉末，ＳｉＯ2 粉末（シリカ），ポリエチ
レン樹脂等の絶縁性微粒子や、電極反応を考慮してカー
ボン粉末等の電子伝導性を有するものであっても良い。The fine particles to be contained in the fine particle slurry must be insoluble in the non-aqueous solvent of the electrolytic solution. Alumina powder, SiO 2 powder (silica), insulating fine particles such as polyethylene resin, and electrode reaction. In consideration of the above, a carbon powder or the like having electron conductivity may be used.
【００２９】但し、カーボン粉末を保護膜に用いる場合
には、これが脱落して電極表面に再付着してしまうと、
活物質層の活物質が脱落して再付着した場合と同様にこ
れが原因して内部ショートが発生する虞れがある。した
がって、このようなカーボン粉末の脱落を確実に防止す
るために、カーボン粉末に対する結着剤の量を接触界面
による孔部形成効果が維持できる範囲で、ある程度大き
くすることが望ましい。例えば、活物質層における結着
剤の含有率の１．５倍の量で、保護膜に結着剤を含有さ
せれは良い。However, when carbon powder is used for the protective film, if it falls off and reattaches to the electrode surface,
As in the case where the active material in the active material layer is dropped and redeposited, this may cause an internal short circuit. Therefore, in order to reliably prevent such carbon powder from falling off, it is desirable to increase the amount of the binder with respect to the carbon powder to some extent within a range in which the effect of forming pores at the contact interface can be maintained. For example, the protective film may contain the binder in an amount 1.5 times the binder content in the active material layer.
【００３０】これら微粒子の粒径は、０．１〜５０μｍ
の範囲であれば差し支えないが、電解液の浸透性，保護
膜の厚みの制御等の観点から、５〜１０μｍであること
が望ましい。The particle size of these fine particles is 0.1 to 50 μm.
However, the thickness is preferably 5 to 10 μm from the viewpoints of permeability of the electrolytic solution, control of the thickness of the protective film, and the like.
【００３１】また、結着剤としては、ポリフッ化ビニリ
デンの他、耐電解液性を有するものであればゴム性の樹
脂等も使用できる。Further, as the binder, in addition to polyvinylidene fluoride, a rubber resin or the like can be used as long as it has resistance to the electrolytic solution.
【００３２】以上、保護膜に用いられる各種材料を例示
したが、このうち絶縁性材料を保護膜に用いる場合に
は、セパレータを排除してこの保護膜にセパレータとし
ての機能も併せ持たせるようにしても良い。これによ
り、セパレータにかかるコストが削減でき生産効率の向
上に有利である。Although various materials used for the protective film have been exemplified above, when an insulating material is used for the protective film, the separator is excluded so that the protective film also has a function as a separator. May be. As a result, the cost of the separator can be reduced, which is advantageous for improving production efficiency.
【００３３】このような多孔性保護膜が設けられる負
極，正極に用いられる負極活物質，正極活物質として
は、この種の非水電解液二次電池において通常用いられ
ているものがいずれも使用可能である。As the negative electrode provided with such a porous protective film, the negative electrode active material used for the positive electrode, and the positive electrode active material, those usually used in this type of non-aqueous electrolyte secondary battery are used. It is possible.
【００３４】例えば、負極活物質としては、リチウム等
のアルカリ金属や、充放電反応に伴いリチウム等のアル
カリ金属をドープ／脱ドープする材料を用いることがで
きる。後者の例としては、ポリアセチレン、ポリピロー
ル等の導電性ポリマー、あるいはコークス、ポリマー
炭、カーボン・ファイバー等の炭素材料を用いることが
できるが、単位体積当りのエネルギー密度が大きい点か
ら、炭素質材料を使用することが望ましい。炭素質材料
としては、熱分解炭素類、コークス類（石油コークス、
ピッチコークス、石炭コークス等）、カーボンブラック
（アセチレンブラック等）、ガラス状炭素、有機高分子
材料焼成体（有機高分子材料を５００℃以上の適当な温
度で不活性ガス気流中、あるいは真空中で焼成したも
の）、炭素繊維等が用いられる。For example, as the negative electrode active material, it is possible to use an alkali metal such as lithium, or a material that is doped / dedoped with an alkali metal such as lithium in association with charge / discharge reaction. As an example of the latter, a conductive polymer such as polyacetylene or polypyrrole, or a carbon material such as coke, polymer carbon, or carbon fiber can be used, but a carbonaceous material is used because of its large energy density per unit volume. It is desirable to use. Carbonaceous materials include pyrolytic carbons, cokes (petroleum coke,
Pitch coke, coal coke, etc.), carbon black (acetylene black, etc.), glassy carbon, organic polymer material fired body (organic polymer material at an appropriate temperature of 500 ° C. or higher in an inert gas stream or in a vacuum) Fired), carbon fiber, etc. are used.
【００３５】一方、正極活物質としては、二酸化マンガ
ン、五酸化バナジウムのような遷移金属酸化物や、硫化
鉄、硫化チタンのような遷移金属カルコゲン化物、さら
にはこれらとリチウムとの複合化合物などを用いること
ができる。特に、高電圧、高エネルギー密度が得られ、
サイクル特性にも優れることから、リチウム・コバルト
複合酸化物やリチウム・コバルト・ニッケル複合酸化物
が望ましい。On the other hand, examples of the positive electrode active material include transition metal oxides such as manganese dioxide and vanadium pentoxide, transition metal chalcogenides such as iron sulfide and titanium sulfide, and composite compounds of these with lithium. Can be used. In particular, high voltage and high energy density are obtained,
Lithium-cobalt composite oxide and lithium-cobalt-nickel composite oxide are preferable because they have excellent cycle characteristics.
【００３６】また、上記電池に使用される電解液として
は、例えばリチウム塩を電解質とし、これを有機溶媒に
溶解した電解液が用いられる。ここで有機溶媒として
は、特に限定されるものではないが、例えばプロピレン
カーボネート、エチレンカーボネート、ジエチルカーボ
ネート、メチルエチルカーボネート、１，２−ジメトキ
シエタン、１，２−ジエトキシエタン、γ−ブチロラク
トン、テトラヒドロフラン、１，３−ジオキソラン、４
−メチル−１，３−ジオキソラン、ジエチルエーテル、
スルホラン、メチルスルホラン、セトニトリル、プロピ
オニトリル等の単独もしくは二種類以上の混合溶媒が使
用できる。As the electrolytic solution used in the battery, for example, an electrolytic solution in which a lithium salt is used as an electrolyte and this is dissolved in an organic solvent is used. Here, the organic solvent is not particularly limited, but for example, propylene carbonate, ethylene carbonate, diethyl carbonate, methyl ethyl carbonate, 1,2-dimethoxyethane, 1,2-diethoxyethane, γ-butyrolactone, tetrahydrofuran. , 1,3-dioxolane, 4
-Methyl-1,3-dioxolane, diethyl ether,
A single solvent or a mixed solvent of two or more kinds such as sulfolane, methylsulfolane, cetonitrile and propionitrile can be used.
【００３７】電解質も従来より公知のものがいずれも使
用でき、ＬｉＣｌＯ4 、ＬｉＡｓＦ 6 、ＬｉＰＦ6 、Ｌ
ｉＢＦ4 、ＬｉＢ（Ｃ6 Ｈ5 ）4 、ＬｉＣｌ、ＬｉＢ
ｒ、ＣＨ3 ＳＯ3 ＬＩ、ＣＦ3 ＳＯ3 Ｌｉ等がある。Any known electrolyte may be used as the electrolyte.
Can be used, LiClOFour, LiAsF 6, LiPF6, L
iBFFour, LiB (C6HFive)Four, LiCl, LiB
r, CH3SO3LI, CF3SO3There are Li and the like.
【００３８】[0038]
【作用】集電体に負極活物質層を積層してなる負極と、
集電体に正極活物質層を積層してなる正極と、非水電解
液を有する非水電解液二次電池において、負極活物質
層，正極活物質層の少なくともいずれかの表面に、厚さ
０．１〜２００μｍの多孔性保護膜を形成すると、活物
質層表面に存在する活物質が保護膜に強固に結合され
る。このような保護膜形成後であれば、電極が電池缶内
に収納されるまでの間に、電極表面に多少の接触があっ
たとしても、表面の活物質が保護膜に強固に結合されて
いるので、活物質が電極から脱落するといったことがな
い。したがって、電極が電池缶内に収納されるまでの間
に、脱落し、電極表面に再付着した活物質によって誘発
される電池の内部ショートが防止される。[Function] A negative electrode formed by laminating a negative electrode active material layer on a current collector,
In a non-aqueous electrolyte secondary battery having a positive electrode in which a positive electrode active material layer is laminated on a current collector and a non-aqueous electrolytic solution, a thickness is formed on at least one surface of the negative electrode active material layer and the positive electrode active material layer. When the porous protective film having a thickness of 0.1 to 200 μm is formed, the active material existing on the surface of the active material layer is firmly bonded to the protective film. After forming such a protective film, the active material on the surface is firmly bonded to the protective film even if there is some contact with the electrode surface before the electrode is housed in the battery can. Therefore, the active material does not fall off the electrode. Therefore, before the electrode is housed in the battery can, the internal short circuit of the battery caused by the active material that has fallen off and redeposited on the electrode surface is prevented.
【００３９】また、この保護膜は、多孔性であるので、
これを形成することで電極の本来の機能，すなわち電解
液中の電解質イオンとの電極反応が妨げられることはな
く、上記効果は電池性能を劣化させることなく獲得され
る。Further, since this protective film is porous,
By forming this, the original function of the electrode, that is, the electrode reaction with the electrolyte ions in the electrolytic solution is not hindered, and the above effect is obtained without degrading the battery performance.
【００４０】[0040]
【実施例】以下、本発明の好適な実施例について実験結
果に基づいて説明する。EXAMPLES Preferred examples of the present invention will be described below based on experimental results.
【００４１】実施例１ 本実施例は活物質層表面に形成する保護膜として不織布
を用いた例である。 Example 1 In this example, a non-woven fabric is used as a protective film formed on the surface of an active material layer.
【００４２】本実施例で作製した非水電解液二次電池の
構成を図１に示す。上記非水電解液二次電池は以下のよ
うにして作製した。The structure of the non-aqueous electrolyte secondary battery produced in this example is shown in FIG. The non-aqueous electrolyte secondary battery was manufactured as follows.
【００４３】まず、負極１は次のようにして作製した。
出発原料として石油ピッチを用い、これを焼成して粗粒
状のピッチコークスを得た。この粗粒状のピッチコーク
スを粉砕して平均粒径２０μｍの粉末とし、この粉末を
不活性ガス中、温度１０００℃で、焼成して不純物を除
去し、コークス材料粉末を生成した。First, the negative electrode 1 was manufactured as follows.
Petroleum pitch was used as a starting material, and this was fired to obtain coarse-grained pitch coke. This coarse-grained pitch coke was crushed into a powder having an average particle size of 20 μm, and the powder was fired in an inert gas at a temperature of 1000 ° C. to remove impurities, thereby producing a coke material powder.
【００４４】このようにして生成したコークス材料粉末
を負極活物質担持体とし、このコークス材料粉末９０重
量部を、結着剤としてポリフッ化ビニリデン（ＰＶｄ
Ｆ）１０重量部と混合し、負極合剤を調製した。この負
極合剤を溶剤であるＮ−メチルピロリドンに分散させて
負極合剤スラリーとした。The coke material powder thus produced was used as a negative electrode active material carrier, and 90 parts by weight of this coke material powder was used as a binder for polyvinylidene fluoride (PVd).
F) 10 parts by weight were mixed to prepare a negative electrode mixture. This negative electrode mixture was dispersed in N-methylpyrrolidone as a solvent to prepare a negative electrode mixture slurry.
【００４５】次に、この負極合剤スラリーを負極集電体
９となる厚さ１０μｍの帯状の銅箔の両面に塗布すると
同時に、塗膜がまだ濡れている状態のうちに、塗膜上に
保護膜となる不織布を載せ、乾燥させた。その結果、表
面に不織布３１が貼り合わされたかたちの負極活物質層
３２が形成された。Next, this negative electrode mixture slurry is applied to both surfaces of a strip-shaped copper foil having a thickness of 10 μm to be the negative electrode current collector 9 and, at the same time, while the coating film is still wet, it is applied onto the coating film. A non-woven fabric as a protective film was placed and dried. As a result, the negative electrode active material layer 32 in the form of the non-woven fabric 31 being attached to the surface was formed.
【００４６】なお、本実施例では、不織布としてマニラ
麻を用いた。このマニラ麻は、１ｍ 2 当たりの重量が１
１ｇ，厚さが４０μｍである。In this embodiment, the non-woven fabric is Manila.
I used hemp. This Manila hemp is 1m 2Weight per hit is 1
The thickness is 1 g and the thickness is 40 μm.
【００４７】そして、このようにして表面に保護膜３１
を有して形成された負極活物質層３２を、ローラプレス
機により圧縮成形することで帯状負極を作製した。な
お、帯状負極１は、成形後の負極活物質層３２の膜厚が
両面共に９０μｍで同一であり、幅が５５．６ｍｍ、長
さが５５１．５ｍｍである。Then, the protective film 31 is formed on the surface in this manner.
The strip-shaped negative electrode was produced by compression-molding the negative electrode active material layer 32 formed by having a roller press. In addition, in the strip-shaped negative electrode 1, the negative electrode active material layer 32 after molding has the same film thickness of 90 μm on both surfaces, the width is 55.6 mm, and the length is 551.5 mm.
【００４８】次に、正極２を次のようにして作製した。
炭酸リチウム０．５モルと炭酸コバルト１モルとを混合
して、空気中、温度９００℃で５時間焼成することによ
ってＬｉＣｏＯ2 を得た。Next, the positive electrode 2 was produced as follows.
LiCoO 2 was obtained by mixing 0.5 mol of lithium carbonate and 1 mol of cobalt carbonate and baking in air at a temperature of 900 ° C. for 5 hours.
【００４９】このＬｉＣｏＯ2 を正極活物質とし、この
ＬｉＣｏＯ2 ９１重量部を、導電剤としてグラファイト
６重量部と結着剤としてＰＶｄＦ３重量部と混合し、正
極合剤を調製した。この正極合剤をＮ−メチルピロリド
ンに分散させて正極合剤スラリーとした。Using this LiCoO 2 as a positive electrode active material, 91 parts by weight of this LiCoO 2 was mixed with 6 parts by weight of graphite as a conductive agent and 3 parts by weight of PVdF as a binder to prepare a positive electrode mixture. This positive electrode mixture was dispersed in N-methylpyrrolidone to prepare a positive electrode mixture slurry.
【００５０】次に、この正極合剤スラリーを正極集電体
１０となる厚さ２０μｍの帯状のアルミニウム箔の両面
に均一の塗布して乾燥することで正極活物質層３３を形
成し、圧縮成形することで帯状正極２を作製した。この
帯状正極２は、成形後の正極活物質層３３の厚さが両面
共に７０μｍで同一であり、幅が５３．６ｍｍ、長さが
５２３．５ｍｍである。Next, this positive electrode mixture slurry is uniformly applied to both surfaces of a strip-shaped aluminum foil having a thickness of 20 μm to be the positive electrode current collector 10 and dried to form the positive electrode active material layer 33, and compression molding is performed. By doing so, the strip positive electrode 2 was produced. The strip-shaped positive electrode 2 has the same thickness of the positive electrode active material layer 33 after molding of 70 μm on both sides, the width is 53.6 mm, and the length is 523.5 mm.
【００５１】以上のようにして作製した帯状負極１と帯
状正極２を、セパレータ３となる厚さ２５μｍ，幅５
８．１ｍｍの微多孔性ポリプロピレンフィルムを介し
て、負極１，セパレータ３，正極２，セパレータ３の順
に積層して４層構造の積層電極体とした。そして、この
積層電極体をその長さ方向に沿って負極１を内側にして
渦巻型に多数回巻回し、さらに最外周に位置するセパレ
ータの端部をテープ２０で固定し、渦巻式電極体を作製
した。この渦巻式電極体は、中心部の中空部分の内径が
３．５ｍｍ、外径が１７．０ｍｍである。The strip-shaped negative electrode 1 and the strip-shaped positive electrode 2 produced as described above are used as a separator 3 with a thickness of 25 μm and a width of 5 μm.
A negative electrode 1, a separator 3, a positive electrode 2, and a separator 3 were laminated in this order via a 8.1 mm microporous polypropylene film to obtain a laminated electrode body having a four-layer structure. Then, this laminated electrode body is spirally wound many times along the length direction with the negative electrode 1 inside, and further the end portion of the separator located at the outermost periphery is fixed with the tape 20 to form the spirally wound electrode body. It was made. In this spiral electrode body, the hollow portion at the center has an inner diameter of 3.5 mm and an outer diameter of 17.0 mm.
【００５２】以上のように作製した渦巻式電極体を、ニ
ッケルメッキを施した鉄製の電池缶５内に収納し、渦巻
式電極体上下両面に絶縁板４を設置した。そして、負極
１及び正極２の集電を行うためにアルミニウム製リード
１２を正極集電体１０から導出して電池蓋７に、ニッケ
ル製負極リード１１を負極集電体９から導出して電池缶
５に溶接した。The spirally wound electrode body manufactured as described above was housed in a nickel-plated iron battery can 5, and insulating plates 4 were placed on the upper and lower surfaces of the spirally wound electrode body. Then, in order to collect the current of the negative electrode 1 and the positive electrode 2, the lead 12 made of aluminum is drawn out from the positive electrode current collector 10 to the battery lid 7, and the negative electrode lead 11 made of nickel is drawn out from the negative electrode current collector 9 to form a battery can. Welded to 5.
【００５３】次に、渦巻式電極体が収納された電池缶５
の中に、プロピレンカーボネートとジエチルカーボネー
トとの等容量混合溶媒にＬｉＰＦ6 を１モル／ｌなる割
合で溶解した非水電解液を５．０ｇ注入して、渦巻式電
極体に含浸させた。Next, the battery can 5 containing the spiral electrode body.
5.0 g of a non-aqueous electrolytic solution prepared by dissolving LiPF 6 in a mixed solvent of equal volume of propylene carbonate and diethyl carbonate at a ratio of 1 mol / l was injected into the solution to impregnate the spirally wound electrode body.
【００５４】そして、アスファルトで表面を塗布した絶
縁封口ガスケット６を介して電池缶５をかしめることで
電池蓋７を固定し、電池内に気密性を保持させ、直径１
８ｍｍ、高さ６５ｍｍの円筒形非水電解液二次電池を作
成した。The battery lid 5 is fixed by caulking the battery can 5 through the insulating sealing gasket 6 whose surface is coated with asphalt, so that the battery can be kept airtight and have a diameter of 1 mm.
A cylindrical non-aqueous electrolyte secondary battery having a size of 8 mm and a height of 65 mm was prepared.
【００５５】実施例２ 本実施例は活物質層表面に形成する保護膜としてコーテ
ィング膜を用いた例である。 Example 2 In this example, a coating film is used as a protective film formed on the surface of the active material layer.
【００５６】負極の負極活物質層及び保護膜の形成を以
下のようにして行うこと以外は実施例１と同様にして非
水電解液二次電池を作成した。但し、ここでは正極の正
極活物質層の厚さを両面共に６５μｍとし、セパレータ
として厚さが１５μｍの微多孔性フィルムを用いた。A non-aqueous electrolyte secondary battery was prepared in the same manner as in Example 1 except that the formation of the negative electrode active material layer and the protective film of the negative electrode was carried out as follows. However, here, the positive electrode active material layer of the positive electrode had a thickness of 65 μm on both sides, and a microporous film having a thickness of 15 μm was used as a separator.
【００５７】すなわち、実施例１と同様にして調製した
負極合剤スラリーを、負極集電体となる銅箔の両面に塗
布，乾燥することで負極活物質層を形成した。That is, a negative electrode active material layer was formed by applying the negative electrode mixture slurry prepared in the same manner as in Example 1 to both surfaces of a copper foil which will be the negative electrode current collector, and drying.
【００５８】一方、平均粒径約１０μｍ程度のアルミナ
粉末７２重量部、結着剤としてＰＶｄＦ３重量部、溶剤
としてＮ−メチルピロリドン２５重量部を混合して、保
護膜材料となる微粒子スラリーを調製した。On the other hand, 72 parts by weight of alumina powder having an average particle size of about 10 μm, 3 parts by weight of PVdF as a binder and 25 parts by weight of N-methylpyrrolidone as a solvent were mixed to prepare a fine particle slurry as a protective film material. .
【００５９】そして、この微粒子スラリーを負極集電体
上に形成された負極活物質層表面に塗布厚２０μｍ程度
で塗布，乾燥し、多孔性保護膜を形成した。次いで、こ
の保護膜が表面に形成された負極活物質層をローラプレ
ス機により圧縮成形して帯状負極を作成した。帯状負極
は、成形後の負極活物質層の膜厚が両面共に８５μｍで
同一である。Then, this fine particle slurry was applied to the surface of the negative electrode active material layer formed on the negative electrode current collector at a coating thickness of about 20 μm and dried to form a porous protective film. Next, the negative electrode active material layer having the protective film formed on its surface was compression-molded by a roller press machine to prepare a strip-shaped negative electrode. The strip-shaped negative electrode has the same thickness of the negative electrode active material layer after molding, which is 85 μm on both surfaces.
【００６０】実施例３ 本実施例は電極活物質層表面に形成する保護膜としてコ
ーティング膜を用い、且つセパレータを排除した例であ
る。 Example 3 This example is an example in which a coating film was used as a protective film formed on the surface of the electrode active material layer, and the separator was omitted.
【００６１】積層電極体を作製するに際して帯状負極と
帯状正極の間にセパレータを介在させず、帯状負極と帯
状正極のみを積層し、負極が内側になるように渦巻き状
に多数回巻回すること以外は実施例２と同様にして非水
電解液二次電池を作成した。但し、この場合も渦巻式電
極体は、中心部の中空部分の内径が３．５ｍｍ、外径が
１７．０ｍｍである。また、負極活物質層の厚さを９０
μｍ，正極活物質層の厚さを７０μｍとした。In producing the laminated electrode body, a separator is not interposed between the strip-shaped negative electrode and the strip-shaped positive electrode, only the strip-shaped negative electrode and the strip-shaped positive electrode are stacked, and the spiral winding is performed many times so that the negative electrode is inside. A nonaqueous electrolyte secondary battery was prepared in the same manner as in Example 2 except for the above. However, in this case as well, in the spiral electrode body, the inner diameter of the hollow portion at the center is 3.5 mm and the outer diameter is 17.0 mm. In addition, the thickness of the negative electrode active material layer is 90
μm, and the thickness of the positive electrode active material layer was 70 μm.
【００６２】比較例 負極活物質層表面に不織布を貼り合わせないこと以外は
実施例１と同様にして非水電解液二次電池を作成した。 Comparative Example A non-aqueous electrolyte secondary battery was prepared in the same manner as in Example 1 except that a non-woven fabric was not attached to the surface of the negative electrode active material layer.
【００６３】以上のようにして作製した各電池につい
て、内部ショートの発生率を調べた。The rate of occurrence of internal short circuit was examined for each battery manufactured as described above.
【００６４】なお、内部ショートの発生率を測定するに
は、作成された電池について、作成後直ちに初充電を行
い、２週間放置した。そして、２週間放置後、開路電圧
を測定し、この電圧が基準以下の電圧を「内部ショート
有り」と判断した。以上のようにして測定した電池の内
部ショートの発生率を表１に示す。In order to measure the rate of occurrence of internal short circuit, the prepared battery was initially charged immediately after preparation and left for 2 weeks. Then, after being left for 2 weeks, the open circuit voltage was measured, and a voltage at which this voltage was lower than the reference was judged to be “with internal short circuit”. Table 1 shows the occurrence rate of the internal short circuit of the battery measured as described above.
【００６５】[0065]
【表１】 [Table 1]
【００６６】表１からわかるように、活物質層表面に保
護膜を形成した実施例１〜実施例３の電池はいずれも比
較例の電池に比べて内部ショートの発生率が低い。この
ことから、活物質層表面に保護膜を形成することは、電
池の内部ショートの発生を抑える上で極めて有効である
ことがわかった。As can be seen from Table 1, all the batteries of Examples 1 to 3 in which the protective film was formed on the surface of the active material layer had a lower occurrence rate of internal short circuit than the batteries of Comparative Example. From this, it was found that forming a protective film on the surface of the active material layer is extremely effective in suppressing the occurrence of internal short circuits in the battery.
【００６７】また、さらに、実施例３の電池は、セパレ
ータを用いていないにもかかわらず、内部ショートが確
実に抑えられており、セパレータがないことで何ら支障
を生じていない。このことから、保護膜として絶縁膜を
用いれば、これをセパレータとして併用することがで
き、セパレータにかかるコストを削減できるといった副
次的効果が得られることがわかった。Further, in the battery of Example 3, the internal short circuit is surely suppressed even though the separator is not used, and the absence of the separator causes no trouble. From this, it was found that if an insulating film is used as the protective film, it can be used together as a separator, and a secondary effect that the cost of the separator can be reduced can be obtained.
【００６８】なお、以上の実施例では、負極のみに保護
膜を形成した場合を例にしているが、勿論、正極のみに
保護膜を形成した場合あるいは負極，正極の両方に保護
膜を形成した場合でも同様の効果が得られる。In the above examples, the case where the protective film is formed only on the negative electrode is taken as an example, but of course, the case where the protective film is formed only on the positive electrode or the protective film is formed on both the negative electrode and the positive electrode. Even in this case, the same effect can be obtained.
【００６９】[0069]
【発明の効果】以上の説明からも明らかなように、本発
明の非水電解液二次電池は、負極活物質層、正極活物質
層のいずれかの表面に厚さ０．１〜２００μｍの多孔性
保護膜が形成されているので、この保護膜によって、活
物質層を形成した後、電極が電池缶内に収納されるまで
の間に発生する活物質の脱落，再付着が防止できる。し
たがって、電極表面に再付着した活物質によって誘発さ
れる電池の内部ショートが防止でき、高い信頼性，安全
性を得ることができる。As apparent from the above description, the non-aqueous electrolyte secondary battery of the present invention has a thickness of 0.1 to 200 μm on either surface of the negative electrode active material layer or the positive electrode active material layer. Since the porous protective film is formed, the protective film can prevent the active material from falling off and redepositing after the active material layer is formed and before the electrode is housed in the battery can. Therefore, an internal short circuit of the battery caused by the active material redeposited on the electrode surface can be prevented, and high reliability and safety can be obtained.
【図１】電極の活物質層上に保護膜として不織布が貼着
された様子を示す模式図である。FIG. 1 is a schematic view showing a state in which a nonwoven fabric is stuck as a protective film on an active material layer of an electrode.
【図２】電極の活物質層上に保護膜として微粒子を含有
するコーティング膜が塗布された様子を示す模式図であ
る。FIG. 2 is a schematic view showing a state in which a coating film containing fine particles is applied as a protective film on an active material layer of an electrode.
【図３】本発明を適用した非水電解液二次電池の一構成
例を示す概略縦断面図である。FIG. 3 is a schematic vertical cross-sectional view showing one structural example of a non-aqueous electrolyte secondary battery to which the present invention is applied.
１ 負極 ２ 正極 ３ セパレータ ９ 負極集電体 １０ 正極集電体 ３１ 多孔性保護膜 ３２ 負極活物質層 ３３ 正極活物質層 1 Negative electrode 2 Positive electrode 3 Separator 9 Negative electrode current collector 10 Positive electrode current collector 31 Porous protective film 32 Negative electrode active material layer 33 Positive electrode active material layer
Claims (3)
る負極と、集電体に正極活物質塗布層を積層してなる正
極と、非水電解液を有する非水電解液二次電池におい
て、 負極活物質塗布層、正極活物質塗布層のいずれかの表面
に厚さ０．１〜２００μｍの多孔性保護膜が形成されて
いることを特徴とする非水電解液二次電池。1. A non-aqueous electrolyte solution having a non-aqueous electrolyte, a negative electrode formed by laminating a negative electrode active material coating layer on a current collector, a positive electrode formed by laminating a positive electrode active material coating layer on a current collector. In the secondary battery, a non-aqueous electrolyte secondary battery in which a porous protective film having a thickness of 0.1 to 200 μm is formed on the surface of either the negative electrode active material coating layer or the positive electrode active material coating layer. .
徴とする請求項１記載の非水電解液二次電池。2. The non-aqueous electrolyte secondary battery according to claim 1, wherein the porous protective film is a non-woven fabric.
からなることを特徴とする請求項１記載の非水電解液二
次電池。3. The non-aqueous electrolyte secondary battery according to claim 1, wherein the porous protective film comprises a resin binder and solid particles.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP01009194A JP3371301B2 (en) | 1994-01-31 | 1994-01-31 | Non-aqueous electrolyte secondary battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP01009194A JP3371301B2 (en) | 1994-01-31 | 1994-01-31 | Non-aqueous electrolyte secondary battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH07220759A true JPH07220759A (en) | 1995-08-18 |
| JP3371301B2 JP3371301B2 (en) | 2003-01-27 |
Family
ID=11740669
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP01009194A Expired - Fee Related JP3371301B2 (en) | 1994-01-31 | 1994-01-31 | Non-aqueous electrolyte secondary battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3371301B2 (en) |
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