JP2000082498A - Nonaqueous electrolyte secondary battery - Google Patents
Nonaqueous electrolyte secondary batteryInfo
- Publication number
- JP2000082498A JP2000082498A JP10250065A JP25006598A JP2000082498A JP 2000082498 A JP2000082498 A JP 2000082498A JP 10250065 A JP10250065 A JP 10250065A JP 25006598 A JP25006598 A JP 25006598A JP 2000082498 A JP2000082498 A JP 2000082498A
- Authority
- JP
- Japan
- Prior art keywords
- positive electrode
- active material
- negative electrode
- electrode active
- 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
-
- 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
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、非水電解液を用い
た二次電池に関するものであり、とくに初期容量の低下
が少ないリチウム電池等の二次電池に関するものであ
る。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a secondary battery using a non-aqueous electrolyte, and more particularly to a secondary battery such as a lithium battery with a small decrease in initial capacity.
【０００２】[0002]
【従来の技術】近年の電子技術のめざましい進歩は、電
子機器の小型、軽量化を次々と実現させている。それに
伴い、携帯用情報端末としての電池に対してもますます
小型、軽量、かつ、高エネルギー密度であることが求め
られている。2. Description of the Related Art In recent years, remarkable progress in electronic technology has enabled electronic devices to be reduced in size and weight one after another. Accordingly, batteries as portable information terminals are required to be smaller and lighter and have higher energy density.
【０００３】従来、二次電池としては、鉛電池、ニッケ
ル−カドミウム電池等の水溶液系電池が主流であった。
しかし、これらの水溶液系電池はサイクル特性に優れる
が、電池重量やエネルギー密度の点では十分満足できる
ものではない。Conventionally, aqueous secondary batteries such as lead batteries and nickel-cadmium batteries have been the mainstream secondary batteries.
However, although these aqueous batteries are excellent in cycle characteristics, they are not sufficiently satisfactory in terms of battery weight and energy density.
【０００４】一方、近年、炭素材料等のリチウムイオン
のドープおよび脱ドープが可能な物質を負極活物質に用
い、リチウム複合金属酸化物を正極に使用する非水電解
液二次電池が開発されている。リチウムイオン電池等の
非水電解液二次電池は、ニッケルカドミウム電池やニッ
ケル水素電池に比べて、容積面でも、重量面でも、高エ
ネルギ密度を有し、自己放電も少なく、軽量である等の
利点を有することから小型の機器用の電池として利用さ
れている。On the other hand, in recent years, a non-aqueous electrolyte secondary battery using a material capable of doping and undoping lithium ions such as a carbon material as a negative electrode active material and using a lithium composite metal oxide for a positive electrode has been developed. I have. Non-aqueous electrolyte secondary batteries such as lithium-ion batteries have higher energy density, lower self-discharge, lighter weight, etc., in terms of volume and weight, compared to nickel cadmium batteries and nickel-metal hydride batteries. Because of its advantages, it is used as a battery for small devices.
【０００５】リチウムイオン電池の製造では、リチウム
をドープした炭素質材料等の入手あるいは取り扱いの問
題から、放電状態にあるリチウムイオンをドープしてい
ない炭素材料と、リチウムと遷移金属の酸化物からなる
リチウム複合酸化物を正極材料として電池を組み立てた
後に、充電することが行われている。In the manufacture of a lithium ion battery, a carbon material which is in a discharged state and which is not doped with lithium ions, and an oxide of lithium and a transition metal are used due to the problem of obtaining or handling a lithium-doped carbonaceous material. 2. Description of the Related Art After a battery is assembled using a lithium composite oxide as a positive electrode material, charging is performed.
【０００６】[0006]
【発明が解決しようとする課題】炭素材料等を負極材料
とした場合、電池の初期充電反応において、正極活物質
中のリチウムが炭素質中にドープされるが、その後の電
池の放電あるいは充電反応では、初期充電によって負極
中にドープされた全リチウム量のうち、８０〜９０％程
度しか負極の炭素材料から脱ドープされず、残余のリチ
ウムは負極から取り出すことができなくなるので、正極
側では初期の量のリチウム複合酸化物を形成することが
できないので、以後のサイクルにおいて、電池容量が大
幅に低下するという問題があった。When a carbon material or the like is used as the negative electrode material, lithium in the positive electrode active material is doped into the carbonaceous material in the initial charge reaction of the battery. In this case, only about 80 to 90% of the total amount of lithium doped in the negative electrode due to the initial charge is dedoped from the carbon material of the negative electrode, and the remaining lithium cannot be removed from the negative electrode. Since the amount of the lithium composite oxide cannot be formed, there is a problem that the battery capacity is significantly reduced in the subsequent cycles.
【０００７】こうした問題点を解決するために、正極活
物質としてＬｉＭＯx （式中、ＭはＣｏ、Ｎｉ、Ｆｅお
よびＭｎのうちから選択される１種又は２種以上の元素
を表す）で示されるリチウム含有複合酸化物に電気化学
的あるいは化学的にリチウムをドープしたものを用いる
ことによってリチウムの量が不足することを防止するこ
とが特開平４−１８１６６０号公報に記載されている。To solve these problems, LiMO x (where M represents one or more elements selected from Co, Ni, Fe and Mn) is used as a positive electrode active material. Japanese Patent Application Laid-Open No. 4-181660 describes that a lithium-containing composite oxide obtained by electrochemically or chemically doping lithium is used to prevent shortage of lithium.
【０００８】また、初期電池容量の落ち込みを減少さ
せ、サイクル特性を向上させるために、正極中もしくは
正極とセパレータの間に、粉末あるいは鱗片状の金属リ
チウムを混入することが特開平９−２１３３７６号公報
において提案されている。In order to reduce the drop in the initial battery capacity and improve the cycle characteristics, powder or flaky metallic lithium is mixed in the positive electrode or between the positive electrode and the separator. It is proposed in the gazette.
【０００９】ところが、これらの方法では、正極活物質
に電気化学的あるいは化学的にリチウムをドープする工
程が必要であったり、あるいはリチウム金属粉末を正極
活物質に混入する工程が必要である。例えば、正極活物
質に電気化学的あるいは化学的にリチウムをドープする
工程は複雑であり生産性を考慮すると現実的ではない。
また、化学的に非常に活性である粉末あるいは鱗片状の
金属リチウムを正極中に混入させることも安全対策上の
手段をとる必要があり工程を複雑なものとする。また、
金属リチウムを正極中に混入させた電池は、安全性上の
問題があり、信頼性の高い非水電解液二次電池を簡便に
製造することは極めて困難であった。However, these methods require a step of electrochemically or chemically doping lithium into the positive electrode active material, or a step of mixing lithium metal powder into the positive electrode active material. For example, the step of electrochemically or chemically doping lithium into the positive electrode active material is complicated and is not realistic in view of productivity.
In addition, it is necessary to take measures for safety measures to mix powder or flaky metallic lithium which is chemically very active into the positive electrode, which complicates the process. Also,
Batteries in which metallic lithium is mixed in the positive electrode have safety problems, and it has been extremely difficult to easily manufacture a highly reliable nonaqueous electrolyte secondary battery.
【００１０】本発明は、金属イオンをドープ、脱ドープ
する正極活物質層および負極活物質層をそれぞれ集電体
上に形成した正極板および負極板をセパレータを介して
巻回した発電要素を有する非水電解液二次電池におい
て、初期充電時に負極中に取り込まれ、後の充放電に寄
与しない非水系電池における初期容量の低下を解決する
ことを課題とするものであり、とくにリチウムをドープ
する負極材料とリチウム含有複合金属酸化物を正極材料
を用いたリチウム電池において、初期充電時に負極中に
取り込まれ、後の充放電に寄与しないリチウムイオンを
補うことによって、初期容量の低下のないリチウム電池
を提供することを課題とするものである。The present invention has a power generating element in which a positive electrode plate and a negative electrode plate each having a positive electrode active material layer and a negative electrode active material layer to be doped and dedoped with metal ions formed on a current collector are wound via a separator. In a non-aqueous electrolyte secondary battery, it is an object to solve a decrease in initial capacity in a non-aqueous battery that is taken into a negative electrode at the time of initial charge and does not contribute to subsequent charge and discharge, and in particular, is doped with lithium. In a lithium battery using a negative electrode material and a lithium-containing composite metal oxide as a positive electrode material, lithium batteries that are taken into the negative electrode during initial charging and that do not contribute to subsequent charge / discharge compensate for lithium ions without a decrease in initial capacity. It is an object to provide
【００１１】[0011]
【課題を解決するための手段】本発明は、金属イオンを
ドープ、脱ドープする正極活物質層および負極活物質層
をそれぞれ集電体上に形成した正極板および負極板をセ
パレータを介して巻回した発電要素を有する非水電解液
二次電池において、正極集電体には、負極容量に対応す
る正極活物質層を形成するともに、負極容量に対応する
正極活物質層の量を超える正極活物質層を、正極集電体
がセパレータを介して対向する隣接する負極板に対向し
ていない領域の正極集電体上に存在させて巻回した非水
電解液二次電池である。According to the present invention, a positive electrode plate and a negative electrode plate each having a positive electrode active material layer and a negative electrode active material layer on which a metal ion is doped and dedoped formed on a current collector are wound via a separator. In a non-aqueous electrolyte secondary battery having a turned power generating element, the positive electrode current collector has a positive electrode active material layer corresponding to the negative electrode capacity and a positive electrode that exceeds the amount of the positive electrode active material layer corresponding to the negative electrode capacity. A nonaqueous electrolyte secondary battery in which an active material layer is wound while being present on the positive electrode current collector in a region where the positive electrode current collector does not face an adjacent negative electrode plate with a separator interposed therebetween.
【００１２】負極容量に対応する正極活物質層の量を超
える正極活物質層を複数個の領域に分けて設けた前記の
非水電解液二次電池である。負極容量に対応する量以上
の正極活物質層が、負極容量の３〜２５％の容量に相当
するものである前記の非水電解液二次電池である。The above non-aqueous electrolyte secondary battery is provided with a positive electrode active material layer having an amount exceeding the amount of the positive electrode active material layer corresponding to the negative electrode capacity provided in a plurality of regions. The nonaqueous electrolyte secondary battery described above, wherein the positive electrode active material layer in an amount equal to or more than the negative electrode capacity corresponds to a capacity of 3 to 25% of the negative electrode capacity.
【００１３】また、金属イオンをドープ、脱ドープする
正極活物質層および負極活物質層をそれぞれ集電体上に
形成した正極板および負極板をセパレータを介して巻回
した発電要素を有する非水電解液二次電池において、正
極集電体には、負極容量に対応した正極活物質層を形成
するともに、正極集電体上に電池反応に関与する金属イ
オンを生成する金属を存在させて巻回した非水電解液二
次電池である。金属イオンがリチウムであり、正極集電
体上に存在させる金属が金属リチウムである前記の非水
電解液二次電池である。Also, a non-aqueous battery having a power generating element in which a positive electrode plate and a negative electrode plate each having a positive electrode active material layer and a negative electrode active material layer for doping and dedoping metal ions formed on a current collector are wound with a separator interposed therebetween. In an electrolyte secondary battery, a positive electrode current collector is formed with a positive electrode active material layer corresponding to the negative electrode capacity, and a metal that generates metal ions involved in a battery reaction is present on the positive electrode current collector and wound. This is a rotated non-aqueous electrolyte secondary battery. The above non-aqueous electrolyte secondary battery in which the metal ion is lithium and the metal present on the positive electrode current collector is lithium metal.
【００１４】正極集電体上に金属リチウムを複数個の領
域に分けて設けた前記の非水電解液二次電池である。正
極集電体上に設ける金属リチウムが、負極容量の３〜２
５％の容量に相当するものである前記の非水電解液二次
電池である。負極活物質が炭素質材料、正極活物質が遷
移金属複合金属酸化物である前記の非水電解液二次電池
である。正極活物質が、マンガン、コバルト、ニッケル
の一種または二種以上を構成要素とするリチウム含有複
合金属酸化物の少なくとも一種を含む前記の非水電解液
二次電池である。The above-mentioned non-aqueous electrolyte secondary battery in which metallic lithium is provided in a plurality of regions on a positive electrode current collector. The metallic lithium provided on the positive electrode current collector has a capacity of 3 to 2 of the negative electrode capacity.
The above non-aqueous electrolyte secondary battery having a capacity of 5%. The above nonaqueous electrolyte secondary battery in which the negative electrode active material is a carbonaceous material and the positive electrode active material is a transition metal composite metal oxide. The nonaqueous electrolyte secondary battery according to the above, wherein the positive electrode active material contains at least one lithium-containing composite metal oxide containing one or more of manganese, cobalt, and nickel as constituent elements.
【００１５】[0015]
【発明の実施の形態】本発明の非水電解液二次電池は、
金属イオンをドープおよび脱ドープする負極材料と、複
合金属酸化物を正極活物質とした電池において、初期充
電において、負極中にドープされて利用されない金属イ
オンを補給することによって電池の初期容量を維持する
ものである。BEST MODE FOR CARRYING OUT THE INVENTION The non-aqueous electrolyte secondary battery of the present invention
Maintain the initial capacity of the battery by replenishing unused metal ions doped in the negative electrode during initial charging in a battery using a negative electrode material doped and dedoped with metal ions and a composite metal oxide as a positive electrode active material. Is what you do.
【００１６】以下に図面を参照して本発明の非水電解液
電池を説明する。図１は、本発明の非水電解液電池の一
実施例を説明する一部を切り欠いた断面図である。ニッ
ケルめっき鋼から形成される電池缶１の上部に、防爆用
の安全装置２を備えた電極ヘッダ３を備えている。電極
ヘッダ３と電池缶１は、ガスケット４により封止されて
いる。第１の絶縁円盤５がガスケット４と電極ヘッダ３
のすぐ下に設けられている細径部６の直下に配置されて
いる。第２の絶縁円盤７が、電池缶１の底部に配置され
ている。正極板８と負極板９とをセパレータ１０を介し
て巻回した発電要素のジェリーロール１１が電池缶１内
に配置されている。正極板から延びる、正極タブ１２
は、電極ヘッダ３に導電接続されており、負極板９に接
続された負極タブ１３は、電池缶１に接続されている。
ジェリーロール１１の巻回は、正極板、セパレータ、負
極板、セパレータの順に重ねて巻回装置の芯に取り付け
て所定の回数の巻回を行っている。巻回の後にジェリー
ロールから芯を取り除くために、中央部には、空洞１４
が形成されている。The non-aqueous electrolyte battery according to the present invention will be described below with reference to the drawings. FIG. 1 is a partially cutaway cross-sectional view illustrating one embodiment of the nonaqueous electrolyte battery of the present invention. An electrode header 3 having an explosion-proof safety device 2 is provided above a battery can 1 made of nickel-plated steel. The electrode header 3 and the battery can 1 are sealed with a gasket 4. The first insulating disk 5 includes the gasket 4 and the electrode header 3
Is disposed immediately below the small-diameter portion 6 provided immediately below. A second insulating disk 7 is arranged at the bottom of the battery can 1. A jelly roll 11 of a power generating element in which a positive electrode plate 8 and a negative electrode plate 9 are wound via a separator 10 is disposed in the battery can 1. Positive electrode tab 12 extending from the positive electrode plate
Are electrically conductively connected to the electrode header 3, and the negative electrode tab 13 connected to the negative electrode plate 9 is connected to the battery can 1.
The jelly roll 11 is wound a predetermined number of times by stacking a positive electrode plate, a separator, a negative electrode plate, and a separator in that order and attaching the jelly roll 11 to a core of a winding device. In order to remove the core from the jelly roll after winding, a hollow 14
Are formed.
【００１７】図５は、ジェリーロールを説明する図であ
り、巻回軸に垂直な面で切断した断面図であり、従来の
電池のジェリーロールを説明する図である。正極板８お
よび負極板９は、正極活物質を含有する組成物層および
負極材料含有組成物層を対向させてセパレータ１０を介
して巻回されており、正極集電体８ａ上の正極活物質層
を形成していない部分に正極タブ１２を接合し、また負
極集電体９ａ上の負極活物質層が形成されていない部分
に負極タブ１３が接合されている。FIG. 5 is a view for explaining the jelly roll, and is a cross-sectional view taken along a plane perpendicular to the winding axis, and is a view for explaining the jelly roll of the conventional battery. The positive electrode plate 8 and the negative electrode plate 9 are wound with a composition layer containing a positive electrode active material and a composition layer containing a negative electrode material facing each other with a separator 10 interposed therebetween. The positive electrode tab 12 is joined to a portion where the layer is not formed, and the negative electrode tab 13 is joined to a portion where the negative electrode active material layer is not formed on the negative electrode current collector 9a.
【００１８】これに対して、本発明のリチウム電池は、
負極活物質層を形成した面に対向していない正極板上
に、正極活物質層あるいは金属リチウム層を設けた電池
である。On the other hand, the lithium battery of the present invention
A battery in which a positive electrode active material layer or a metal lithium layer is provided on a positive electrode plate which is not opposed to a surface on which a negative electrode active material layer is formed.
【００１９】図２は、本発明の一実施例の電池のジェリ
ーロールを説明する図である。図２（Ａ）は、正極板８
の巻はじめ部を負極板よりもずらして巻始めることによ
って、正極板に接するセパレータ１０の反対側には負極
板９が存在しない部分８ｂを設け、正極活物質層８ｃを
存在させたものであり、巻始め部の正極活物質層を形成
していない正極集電体８ａ上に、正極タブ１２を接続し
たものであり、負極板９には、負極タブ１３を接続した
ジェリーロール１１である。FIG. 2 is a diagram illustrating a jelly roll of a battery according to one embodiment of the present invention. FIG. 2A shows the positive electrode plate 8.
The winding start portion is shifted from the negative electrode plate to start winding, so that a portion 8b where the negative electrode plate 9 does not exist is provided on the opposite side of the separator 10 in contact with the positive electrode plate, and the positive electrode active material layer 8c is present. A positive electrode tab 12 is connected to a positive electrode current collector 8 a on which a positive electrode active material layer is not formed at the beginning of winding, and a jelly roll 11 to which a negative electrode tab 13 is connected is connected to a negative electrode plate 9.
【００２０】また、図２（Ｂ）は、正極板８の巻はじめ
部を負極板よりもずらして巻始めるとともに、正極板に
接するセパレータの反対側には負極板が存在しない部分
８ｂを設け、正極板の一方の面のみに正極活物質層８ｃ
を存在させたものであり、巻始め部の正極活物質を含有
する組成物層を形成していない正極集電体８ａ上に、正
極タブ１２を接続したものである。FIG. 2B shows that the winding start portion of the positive electrode plate 8 is shifted from the negative electrode plate to start winding, and a portion 8b where the negative electrode plate does not exist is provided on the opposite side of the separator in contact with the positive electrode plate. The positive electrode active material layer 8c is formed only on one surface of the positive electrode plate.
The positive electrode tab 12 is connected to the positive electrode current collector 8a at the beginning of the winding where the composition layer containing the positive electrode active material is not formed.
【００２１】図２（Ｃ）は、正極板８の巻始め部に、活
物質を含有する組成物層を形成していない正極タブ１２
の接続用の正極集電体８ａを設けるとともに、巻始め部
の負極板とセパレータを介して対向する面には、正極活
物質層を形成しない部分８ｄを設けたものであり、正極
板の正極活物質層を形成しない部分８ｄの裏面には、負
極容量に対応する量を超える正極活物質層８ｃを形成す
るしたものであり、図２（Ａ）あるいは図２（Ｂ）と同
様の効果を奏する。FIG. 2C shows a positive electrode tab 12 having no active material-containing composition layer formed at the beginning of winding of the positive electrode plate 8.
A positive electrode current collector 8a for connection is provided, and a portion 8d on which a positive electrode active material layer is not formed is provided on a surface facing the negative electrode plate at the beginning of winding via a separator. The positive electrode active material layer 8c exceeding the amount corresponding to the negative electrode capacity is formed on the back surface of the portion 8d where the active material layer is not formed, and the same effect as that of FIG. 2A or FIG. 2B is obtained. Play.
【００２２】また、図３は、本発明の他の実施例の電池
のジェリーロールを説明する図である。図３（Ａ）は、
正極板８の巻終わりの部分の正極集電体８ａの負極板９
に対向しない部分８ｂに、正極活物質層８ｃを存在させ
たものである。 図３（Ｂ）は、負極板に対応しない部
分の正極集電体８ａ上の一方の面のみに正極活物質層を
形成して巻回したものである。FIG. 3 is a view for explaining a jelly roll of a battery according to another embodiment of the present invention. FIG. 3 (A)
Negative electrode plate 9 of positive electrode current collector 8a at the end of winding of positive electrode plate 8
The positive electrode active material layer 8c is present in a portion 8b that does not face the positive electrode. FIG. 3B illustrates a structure in which a positive electrode active material layer is formed and wound only on one surface of the positive electrode current collector 8a in a portion not corresponding to the negative electrode plate.
【００２３】また、図４は、本発明の他の実施例の電池
のジェリーロールを説明する図である。図４は、正極集
電体上に金属リチウムを存在させたものであり、図４
（Ａ）は、正極板の巻始め部の正極集電体８ａ上に金属
リチウム１５を存在させたものであり、図４（Ｂ）は、
正極集電体８ａの巻始め部と巻終わり部の両者に金属リ
チウムを存在させたものである。FIG. 4 is a view for explaining a jelly roll of a battery according to another embodiment of the present invention. FIG. 4 shows the case where metallic lithium is present on the positive electrode current collector.
FIG. 4A shows that the metallic lithium 15 is present on the positive electrode current collector 8a at the beginning of the winding of the positive electrode plate, and FIG.
This is one in which metallic lithium is present in both the winding start portion and the winding end portion of the positive electrode current collector 8a.
【００２４】本発明の非水電解液二次電池において、正
極活物質としては、リチウム、ナトリウム等のアルカリ
金属とコバルト、ニッケル、マンガン等の遷移金属から
なるリチウムイオンをドープおよび脱ドープする複合金
属酸化物を用いることができる。負極活物質としては、
リチウムイオンをドープおよび脱ドープするコークス、
グラファイト、黒鉛化メソカーボンマイクロビーズ、黒
鉛化炭素繊維、黒鉛前駆体炭素、非晶質炭素等の炭素質
材料、遷移金属複合酸化物等を用いることができる。In the nonaqueous electrolyte secondary battery of the present invention, the positive electrode active material is a composite metal which is doped and dedoped with lithium ions comprising an alkali metal such as lithium and sodium and a transition metal such as cobalt, nickel and manganese. An oxide can be used. As the negative electrode active material,
Coke for doping and undoping lithium ions,
Graphite, graphitized mesocarbon microbeads, graphitized carbon fibers, graphite precursor carbon, carbonaceous materials such as amorphous carbon, transition metal composite oxides, and the like can be used.
【００２５】本発明において、正極板上に設ける負極容
量に対応する量以上の正極活物質、あるいは金属リチウ
ム量は負極容量に対して３〜２５％の放電容量に相当す
る量であることがであることが好ましい。３％未満であ
るとサイクル容量維持の向上が認められず、２５％を超
えると充電時に負極上に金属リチウムの析出が顕著とな
るため安全性が好ましくない。また、負極容量に対応す
る量以上の正極活物質、あるいは金属リチウムは、一箇
所に配置する方法に限らず複数の箇所に配置しても良
い。In the present invention, the amount of the positive electrode active material or the amount of lithium metal which is equal to or more than the amount corresponding to the negative electrode capacity provided on the positive electrode plate may be an amount corresponding to a discharge capacity of 3 to 25% of the negative electrode capacity. Preferably, there is. If it is less than 3%, no improvement in cycle capacity maintenance is observed, and if it exceeds 25%, the precipitation of metallic lithium on the negative electrode during charging becomes remarkable, which is not preferable in terms of safety. Further, the amount of the positive electrode active material or metallic lithium which is equal to or more than the amount corresponding to the negative electrode capacity is not limited to the method of arranging at one place, but may be arranged at a plurality of places.
【００２６】[0026]
【作用】本発明になる非水電解液二次電池は、負極集電
体上にリチウムをドープおよび脱ドープする負極材料を
含有した負極活物質層を形成した負極板と、正極集電体
上にリチウム含有複合金属酸化物からなる正極活物質層
を形成した正極板とを巻回した発電要素を電池缶に収容
した電池において、正極集電体には、負極容量に対応し
た正極活物質層を形成するともに、負極容量に対応する
以上の量の正極活物質層を、正極板のセパレータを介し
て隣接する負極板に対向していない領域に存在させて巻
回するか、もしくは正極集電体上に金属リチウムを存在
させて巻回したので、初期充放電反応において、負極中
に取り込まれて容量に寄与しないリチウムを補うことに
より、容量容量低下率が少ない電池を提供することがで
きる。The nonaqueous electrolyte secondary battery according to the present invention comprises a negative electrode plate having a negative electrode active material layer containing a negative electrode material for doping and dedoping lithium on a negative electrode current collector; In a battery in which a power generation element wound with a positive electrode plate on which a positive electrode active material layer made of a lithium-containing composite metal oxide is formed is housed in a battery can, the positive electrode current collector has a positive electrode active material layer corresponding to the negative electrode capacity. And then winding the positive electrode active material layer in an area not facing the adjacent negative electrode plate through the separator of the positive electrode plate in an amount larger than the amount corresponding to the negative electrode capacity, Since the metal lithium is wound on the body, the lithium which is taken into the negative electrode and does not contribute to the capacity in the initial charge / discharge reaction is supplemented, whereby a battery with a small capacity capacity reduction rate can be provided.
【００２７】[0027]
【実施例】以下に実施例を示し本発明を説明する。 実施例１ メソフェーズ系炭素材料粉末を負極活物質の９０重量部
と結着材としてポリフッ化ビニリデン（ＰＶＤＦ）１０
重量部を混合し、負極合剤を調整した。そして、この負
極合剤をＮ−メチル２−ピロリドン溶剤に分散させて負
極合剤スラリーを得た。得られた負極合剤スラリーを負
極集電体となる厚さ１０μｍ、幅５７ｍｍ、長さ５３０
ｍｍの帯状銅箔の両面に塗布、乾燥させた後圧縮形成し
て合剤厚さを両面共に８０μｍとした帯状負極板を作製
した。The present invention will be described below with reference to examples. Example 1 90 parts by weight of a mesophase-based carbon material powder and a polyvinylidene fluoride (PVDF) 10 as a binder were used as a binder.
The parts by weight were mixed to prepare a negative electrode mixture. Then, this negative electrode mixture was dispersed in an N-methyl 2-pyrrolidone solvent to obtain a negative electrode mixture slurry. The obtained negative electrode mixture slurry is used as a negative electrode current collector, with a thickness of 10 μm, a width of 57 mm, and a length of 530.
After coating and drying on both sides of a strip of copper foil having a thickness of 80 mm, the strip was formed by compression to prepare a strip-shaped negative electrode plate having a mixture thickness of 80 μm on both sides.
【００２８】炭酸リチウムと二酸化マンガンを混合し、
空気中、温度７８０℃で１２時間焼成して、ＬｉＭｎ2
Ｏ4を得た。このＬｉＭｎ2Ｏ4を正極活物質とし、これ
を９２重量部、導電剤としてグラファイト５重量部、結
着剤としてポリフッ化ビニリデン３重量部を混合し、正
極合剤を調整した。そして、この正極合剤をＮ−メチル
２−ピロリドンを分散させて正極合剤スラリーにした。Mixing lithium carbonate and manganese dioxide,
Baking in air at 780 ° C. for 12 hours to obtain LiMn 2
O 4 was obtained. This LiMn 2 O 4 was used as a positive electrode active material, and 92 parts by weight of this was mixed with 5 parts by weight of graphite as a conductive agent and 3 parts by weight of polyvinylidene fluoride as a binder to prepare a positive electrode mixture. Then, this positive electrode mixture was dispersed in N-methyl 2-pyrrolidone to form a positive electrode mixture slurry.
【００２９】この正極合剤スラリーを正極集電体となる
厚さ２５μｍの帯状アルミニウム箔の両面に均一に塗
布、乾燥させた後、圧縮形成して帯状正極を作製した。
なお、帯状正極は合剤厚さを両面共に１００μｍで同一
とし、幅を５５ｍｍ、長さを４８０ｍｍとした。以上の
ようにして作製した帯状負極板と帯状正極板を厚さ２５
μｍ、幅４１ｍｍを微多孔性ポリプロピレンフィルムよ
りなるセパレータ３を介して負極、セパレータ、正極、
セパレータの順に積層し、多数回巻回した。The positive electrode mixture slurry was uniformly applied to both sides of a 25 μm-thick aluminum foil foil serving as a positive electrode current collector, dried, and then compression-formed to produce a positive electrode strip.
The band-shaped positive electrode had the same mixture thickness of 100 μm on both sides, and had a width of 55 mm and a length of 480 mm. The strip-shaped negative electrode plate and the strip-shaped positive electrode plate manufactured as described above were
A negative electrode, a separator, a positive electrode, a separator having a width of 41 μm and a width of 41 mm made of a microporous polypropylene film.
The layers were laminated in the order of the separator and wound many times.
【００３０】図２（Ａ）に示すように、巻回始めにおい
て、正極板、負極板が対向する部分よりも巻始め側に正
極板のみを１０ｍｍ先に巻回した。このように巻芯に積
層体を巻回した後、最外周に位置するセパレータの最終
端部を幅１５ｍｍの粘着テープによってジェリーロール
に固定した。そして、巻芯をジェリーロールから抜き取
ることにより発電要素を作製した。As shown in FIG. 2A, at the beginning of winding, only the positive electrode plate was wound 10 mm ahead of the portion where the positive and negative electrode plates face each other. After the laminate was wound around the core in this way, the final end of the separator located at the outermost periphery was fixed to a jelly roll with an adhesive tape having a width of 15 mm. Then, a power generating element was prepared by extracting the core from the jelly roll.
【００３１】この発電要素をニッケルめっきが施された
軟鋼製電池缶に収納し、発電要素の上下両面に絶縁板を
配置した。次いで、正極集電体の端部に溶接された厚さ
０．１ｍｍ、幅３ｍｍのアルミニウム製正極タブを電池
蓋に、負極集電体の端部に溶接された厚さ０．１ｍｍ、
幅３ｍｍのニッケル製負極タブを電池缶に溶接し、エチ
レンカーボネート３０重量部とジエチルカーボネート７
０重量部の混合溶液中にＬｉＰＦ6 を１モル／ｌの割合
で溶解した電解液を注入し、電池蓋と電池缶をかしめに
より固定して、直径１８ｍｍ、高さ６５ｍｍの円筒型非
水電解液二次電池を作製した。The power generating element was housed in a nickel-plated mild steel battery can, and insulating plates were arranged on both upper and lower surfaces of the power generating element. Next, a 0.1 mm thick aluminum positive electrode tab having a thickness of 3 mm and a width of 3 mm welded to the end of the positive electrode current collector was used as a battery lid, and a 0.1 mm thickness welded to the end of the negative electrode current collector was used.
A nickel negative electrode tab having a width of 3 mm was welded to the battery can, and 30 parts by weight of ethylene carbonate and diethyl carbonate 7 were welded.
An electrolyte obtained by dissolving LiPF 6 at a ratio of 1 mol / l into 0 parts by weight of the mixed solution was injected, and the battery lid and the battery can were fixed by caulking to form a cylindrical nonaqueous electrolyte having a diameter of 18 mm and a height of 65 mm. A liquid secondary battery was manufactured.
【００３２】得られた電池を充電電流０．５Ａで定電流
充電を行い、電池電圧が４．２Ｖから定電圧充電に切り
替えて定電流充電開始からの総充電時間が２．５時間で
充電を終了した後、放電終止電圧３．０Ｖの条件で放電
を行う充放電サイクルを２００回繰り返し、容量変化を
測定し、その結果を図６に示した。The obtained battery was charged at a constant current of 0.5 A with a charging current of 0.5 A, and the battery voltage was switched from 4.2 V to a constant voltage charge to charge the battery with a total charge time of 2.5 hours from the start of the constant current charge. After the termination, the charge / discharge cycle for discharging under the condition of the discharge end voltage of 3.0 V was repeated 200 times, and the change in capacity was measured. The result is shown in FIG.
【００３３】実施例２ 充放電容量が等しい正極板と負極板を対向させて巻始め
ると共に、負極容量に対して、５、１０、１５、２０、
２５および３０％の容量の金属リチウムを正極集電体上
に設けた点を除き実施例１と同様にリチウム電池を作製
して、実施例１と同様の条件で充放電を繰り返し、初期
充放電容量に対する２００サイクル目の充放電容量を容
量維持率として図７に示した。Example 2 A positive electrode plate and a negative electrode plate having the same charge / discharge capacity were started facing each other, and 5, 10, 15, 20,
A lithium battery was prepared in the same manner as in Example 1 except that lithium metal having a capacity of 25 and 30% was provided on the positive electrode current collector, and charging and discharging were repeated under the same conditions as in Example 1, and initial charging and discharging were performed. The charge / discharge capacity at the 200th cycle with respect to the capacity is shown in FIG. 7 as the capacity retention ratio.
【００３４】比較例１ 正極板と負極板を等しい充放電容量とするとともに、正
極板と負極板が対向する箇所以外には正極活物質あるい
はリチウム金属を配置しないことを除き実施例１と同様
にしてリチウム電池を作製して、実施例１と同様に充放
電を繰り返し、充放電容量の変化を図６に示した。Comparative Example 1 The same procedure as in Example 1 was carried out except that the positive electrode plate and the negative electrode plate had the same charge / discharge capacity, and that no positive electrode active material or lithium metal was provided except where the positive electrode plate and the negative electrode plate faced each other. Thus, a lithium battery was manufactured, and charge and discharge were repeated in the same manner as in Example 1. The change in charge and discharge capacity was shown in FIG.
【００３５】[0035]
【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では、渦巻電極群の対向する正
負極電極以外の正極集電体上に金属リチウムを備えた
り、あるいは渦巻電極群の対向する正負極電極以外に正
極部を配置することで、初期における放電容量の落ち込
みを落ち込みを抑えてサイクル特性を向上できる電池が
得られる。As is clear from the above description, in the nonaqueous electrolyte secondary battery of the present invention, metallic lithium is provided on the positive electrode current collector other than the positive and negative electrodes facing the spiral electrode group, Alternatively, by arranging a positive electrode portion other than the positive and negative electrodes facing the spiral electrode group, it is possible to obtain a battery that can suppress the drop in the initial discharge capacity and improve the cycle characteristics.
【図１】図１は、本発明の非水電解液電池の一実施例を
説明する一部を切り欠いた断面図である。FIG. 1 is a partially cutaway cross-sectional view illustrating one embodiment of a nonaqueous electrolyte battery of the present invention.
【図２】図２は、本発明の一実施例の電池のジェリーロ
ールを説明する図である。FIG. 2 is a diagram illustrating a jelly roll of a battery according to one embodiment of the present invention.
【図３】図３は、本発明の他の実施例の電池のジェリー
ロールを説明する図である。FIG. 3 is a diagram illustrating a jelly roll of a battery according to another embodiment of the present invention.
【図４】図４は、本発明の他の実施例の電池のジェリー
ロールを説明する図である。FIG. 4 is a diagram illustrating a jelly roll of a battery according to another embodiment of the present invention.
【図５】図５は、従来の電池のジェリーロールを説明す
る図である。FIG. 5 is a diagram illustrating a jelly roll of a conventional battery.
【図６】図６は、本発明の実施例１と比較例１の電池の
サイクル特性を示す特性図である。FIG. 6 is a characteristic diagram showing cycle characteristics of the batteries of Example 1 of the present invention and Comparative Example 1.
【図７】図７は、本発明の実施例２における電池の容量
維持率を示す特性図である。FIG. 7 is a characteristic diagram showing a capacity retention ratio of a battery in Example 2 of the present invention.
１…電池缶、２…防爆用の安全装置、３…電極ヘッダ、
４…ガスケット、５…絶縁円盤、６…細径部、７…２の
絶縁円盤、８…正極板、８ａ…正極集電体、８ｂ…セパ
レータの反対側には負極板が存在しない部分、８ｃ…正
極活物質層、８ｄ…正極活物質層が存在しない部分、９
…負極板、１０…セパレータ、１１…ジェリーロール、
１２…正極タブ、１３…負極タブ、１４…空洞、１５…
金属リチウム1 ... battery can, 2 ... explosion-proof safety device, 3 ... electrode header,
4 ... gasket, 5 ... insulating disc, 6 ... small diameter section, 7 ... 2 insulating disc, 8 ... positive electrode plate, 8a ... positive electrode current collector, 8b ... part where no negative electrode plate exists on the side opposite to the separator, 8c ... Positive electrode active material layer, 8d ... Part where no positive electrode active material layer exists, 9
... negative electrode plate, 10 ... separator, 11 ... jelly roll,
12 ... Positive electrode tab, 13 ... Negative electrode tab, 14 ... Cavity, 15 ...
Metal lithium
───────────────────────────────────────────────────── フロントページの続き (72)発明者 粂内 友一 東京都港区芝五丁目７番１号 日本電気株 式会社内 Ｆターム(参考） 5H003 AA04 BB02 BB05 BC05 BD03 5H014 AA04 CC01 HH01 5H029 AJ05 AK03 AL06 BJ02 BJ14 DJ04 HJ01 ──────────────────────────────────────────────────続 き Continuing on the front page (72) Inventor Yuichi Kumeuchi 5-7-1 Shiba, Minato-ku, Tokyo NEC Corporation F-term (reference) 5H003 AA04 BB02 BB05 BC05 BD03 5H014 AA04 CC01 HH01 5H029 AJ05 AK03 AL06 BJ02 BJ14 DJ04 HJ01
Claims (9)
活物質層および負極活物質層をそれぞれ集電体上に形成
した正極板および負極板をセパレータを介して巻回した
発電要素を有する非水電解液二次電池において、正極集
電体には、負極容量に対応する正極活物質層を形成する
ともに、負極容量に対応する正極活物質層の量を超える
正極活物質層を、正極集電体がセパレータを介して対向
する隣接する負極板に対向していない領域の正極集電体
上に存在させて巻回したことを特徴とする非水電解液二
次電池。1. A non-aqueous device having a power generating element in which a positive electrode plate and a negative electrode plate each having a positive electrode active material layer and a negative electrode active material layer to be doped and de-doped with metal ions formed on a current collector are wound via a separator. In an electrolyte secondary battery, a positive electrode current collector is provided with a positive electrode active material layer corresponding to the negative electrode capacity and a positive electrode active material layer exceeding the amount of the positive electrode active material layer corresponding to the negative electrode capacity. A non-aqueous electrolyte secondary battery in which a body is present and wound on a positive electrode current collector in a region not opposed to an adjacent negative electrode plate which is opposed via a separator.
超える正極活物質層を複数個の領域に分けて設けたこと
を特徴とする請求項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 a positive electrode active material layer exceeding the amount of the positive electrode active material layer corresponding to the negative electrode capacity is provided in a plurality of regions.
層が、負極容量の３〜２５％の容量に相当するものであ
ることを特徴とする請求項１ないし２のいずれかに記載
の非水電解液二次電池。3. The method according to claim 1, wherein the amount of the positive electrode active material layer equal to or more than the amount corresponding to the negative electrode capacity corresponds to a capacity of 3 to 25% of the negative electrode capacity. Non-aqueous electrolyte secondary battery.
活物質層および負極活物質層をそれぞれ集電体上に形成
した正極板および負極板をセパレータを介して巻回した
発電要素を有する非水電解液二次電池において、正極集
電体には、負極容量に対応した正極活物質層を形成する
ともに、正極集電体上に電池反応に関与する金属イオン
を生成する金属を存在させて巻回したことを特徴とする
非水電解液二次電池。4. A non-aqueous battery having a power generation element in which a positive electrode plate and a negative electrode plate each having a positive electrode active material layer and a negative electrode active material layer to be doped and de-doped with metal ions formed on a current collector are wound via a separator. In an electrolyte secondary battery, a positive electrode current collector is formed with a positive electrode active material layer corresponding to the negative electrode capacity, and a metal that generates metal ions involved in a battery reaction is present on the positive electrode current collector and wound. A non-aqueous electrolyte secondary battery characterized by being turned.
体上に存在させる金属が金属リチウムであることを特徴
とする請求項４記載の非水電解液二次電池。5. The non-aqueous electrolyte secondary battery according to claim 4, wherein the metal ion is lithium and the metal present on the positive electrode current collector is lithium metal.
領域に分けて設けたことを特徴とする請求項５記載の非
水電解液二次電池。6. The non-aqueous electrolyte secondary battery according to claim 5, wherein metallic lithium is provided on the positive electrode current collector in a plurality of regions.
負極容量の３〜２５％の容量に相当するものであること
を特徴とする請求項５ないし６のいずれかに記載の非水
電解液二次電池。7. The metal lithium provided on the positive electrode current collector,
The non-aqueous electrolyte secondary battery according to any one of claims 5 to 6, which corresponds to a capacity of 3 to 25% of the capacity of the negative electrode.
遷移金属複合金属酸化物であることを特徴とする請求項
１ないし７のいずれかに記載の非水電解液二次電池。8. The non-aqueous electrolyte secondary battery according to claim 1, wherein the negative electrode active material is a carbonaceous material and the positive electrode active material is a transition metal composite metal oxide.
ッケルの一種または二種以上を構成要素とするリチウム
含有複合金属酸化物の少なくとも一種を含むことを特徴
とする請求項１ないし８のいずれかに記載の非水電解液
二次電池。9. The positive electrode active material contains at least one of lithium-containing composite metal oxides containing one or more of manganese, cobalt, and nickel as constituent elements. 3. The non-aqueous electrolyte secondary battery according to 1.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP10250065A JP3033563B2 (en) | 1998-09-03 | 1998-09-03 | Non-aqueous electrolyte secondary battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP10250065A JP3033563B2 (en) | 1998-09-03 | 1998-09-03 | Non-aqueous electrolyte secondary battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JP2000082498A true JP2000082498A (en) | 2000-03-21 |
| JP3033563B2 JP3033563B2 (en) | 2000-04-17 |
Family
ID=17202290
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP10250065A Expired - Lifetime JP3033563B2 (en) | 1998-09-03 | 1998-09-03 | Non-aqueous electrolyte secondary battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3033563B2 (en) |
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