JP2001338639A - Non-aqueous electrolyte battery - Google Patents
Non-aqueous electrolyte batteryInfo
- Publication number
- JP2001338639A JP2001338639A JP2000155401A JP2000155401A JP2001338639A JP 2001338639 A JP2001338639 A JP 2001338639A JP 2000155401 A JP2000155401 A JP 2000155401A JP 2000155401 A JP2000155401 A JP 2000155401A JP 2001338639 A JP2001338639 A JP 2001338639A
- Authority
- JP
- Japan
- Prior art keywords
- positive electrode
- active material
- electrode active
- aqueous electrolyte
- battery
- 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
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、正極活物質を含有
する正極活物質層を備える正極と、負極活物質を含有す
る負極と、非水電解質とを備える非水電解質電池に関す
る。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a non-aqueous electrolyte battery including a positive electrode having a positive electrode active material layer containing a positive electrode active material, a negative electrode containing a negative electrode active material, and a non-aqueous electrolyte.
【０００２】[0002]
【従来の技術】近年、カメラ一体型のＶＴＲ、携帯電
話、ラップトップ型のコンピュータ等の携帯可能な電子
機器や通信機器の小型化及び軽量化が進行しており、こ
れらの駆動用電源として用いられる電池に対しても、小
型化及び軽量化が求められている。これに伴い、電池の
エネルギー密度の向上を目指した研究開発が活発に行わ
れている。2. Description of the Related Art In recent years, portable electronic devices and communication devices such as a camera-integrated VTR, a mobile phone, and a laptop computer have been reduced in size and weight, and are used as power sources for driving these devices. There is also a demand for smaller and lighter batteries. Along with this, research and development aimed at improving the energy density of batteries are being actively conducted.
【０００３】携帯可能な電子機器や通信機器の駆動用電
源としては、従来よりニッケルカドミウム電池や鉛電池
等が使用されているが、これらの水溶液系電解液二次電
池と比較してエネルギー密度がより大きい電池であるリ
チウムイオン二次電池が注目されている。Conventionally, nickel cadmium batteries, lead batteries, and the like have been used as power sources for driving portable electronic devices and communication devices, but their energy density is lower than those of aqueous electrolyte secondary batteries. Attention has been paid to lithium ion secondary batteries, which are larger batteries.
【０００４】リチウムイオン二次電池は、放電電圧が高
く、自己放電が少なく、且つサイクル特性が良好で、高
エネルギー密度であるという優れた特長を有しているの
で、様々な電子機器の電源として使用されつつあり、幅
広い分野に適用可能な電池として期待が高い。[0004] Lithium ion secondary batteries have excellent features of high discharge voltage, low self-discharge, good cycle characteristics, and high energy density, so that they can be used as power sources for various electronic devices. The batteries are being used and are expected to be applicable to a wide range of fields.
【０００５】[0005]
【発明が解決しようとする課題】ところで、リチウムイ
オン二次電池は、その使用用途が多様化するにつれて使
用条件が多岐にわたり、異常な条件下で使用される可能
性が増加している。例えば電池が押しつぶされて電極が
変形したり、又は電池に金属物が刺さることがある。こ
のような場合、電池内部では電極のショートが生じてし
まう。The use conditions of lithium ion secondary batteries have been diversified as their uses have been diversified, and the possibility of use under abnormal conditions has increased. For example, the battery may be crushed to deform the electrodes, or a metal object may be stabbed in the battery. In such a case, the electrodes are short-circuited inside the battery.
【０００６】リチウムイオン二次電池の正極活物質は、
Ｌｉが脱離した状態である充電時に電極のショート等に
より加熱された場合、有機電解液との化学反応に由来す
る発熱を引き起こすことがSolid State Ionics69(1994)
265 J.R.Dahnらの報告により広く知られている。つま
り、電池内部で電極のショートが生じて電極が加熱され
ると、電池は高熱を発する可能性がある。The positive electrode active material of a lithium ion secondary battery is
When heated due to short-circuiting of the electrodes during charging when Li is desorbed, Solid State Ionics69 (1994) may cause heat generation due to a chemical reaction with the organic electrolyte.
265 Known widely by reports by JR Dahn et al. In other words, when the electrodes are short-circuited inside the battery and the electrodes are heated, the battery may generate high heat.
【０００７】そこで、電池が押しつぶされたとしても電
極が変形し難いように、電極を金属製の容器に収納して
いる。また、電池の保護装置として温度ヒューズ、ＰＴ
Ｃ素子、電流ヒューズ等を電池内部に配設することで安
全性を確保している。Therefore, the electrodes are housed in a metal container so that the electrodes are not easily deformed even if the battery is crushed. In addition, thermal fuse, PT
The safety is ensured by disposing a C element, a current fuse and the like inside the battery.
【０００８】その一方で、更なる安全性の確保を目指し
て、非水電解質電池は、種々の条件下における電池の安
定性の向上をより一層求められている。On the other hand, in order to further secure safety, non-aqueous electrolyte batteries are required to further improve the stability of the batteries under various conditions.
【０００９】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、電極が変形をするような異常な状
況下で使用されて、ショートが生じるといった不測の事
態に陥った場合でも、安定性に優れる非水電解質電池を
提供することを目的とする。The present invention has been proposed in view of such a conventional situation. Even when the electrode is used under an abnormal situation where the electrode is deformed, an unexpected situation such as a short circuit occurs. It is an object of the present invention to provide a non-aqueous electrolyte battery having excellent stability.
【００１０】[0010]
【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、本発明に係る非水電解質電池は、正極活物質を含
有する正極活物質層が正極集電体上に複数積層されてい
る正極と、負極活物質を含有する負極と、非水電解質と
を備え、正極活物質層に含有される正極活物質の組成
は、その厚み方向において異なることを特徴とする。In order to achieve the above object, a nonaqueous electrolyte battery according to the present invention has a plurality of positive electrode active material layers containing a positive electrode active material laminated on a positive electrode current collector. A positive electrode, a negative electrode containing a negative electrode active material, and a nonaqueous electrolyte are provided, and the composition of the positive electrode active material contained in the positive electrode active material layer is different in the thickness direction.
【００１１】以上のように構成された本発明に係る非水
電解質電池は、正極活物質の組成がその厚み方向におい
て異なる正極活物質層が正極集電体上に複数積層された
正極を備えるので、ショートが生じるといった不測の事
態に陥った場合でも、正極活と非水電解質との化学反応
による発熱の時間的及び空間的な集中を防止されてい
る。[0011] The nonaqueous electrolyte battery according to the present invention having the above-described structure includes a positive electrode in which a plurality of positive electrode active material layers having different compositions in the thickness direction of the positive electrode active material are laminated on the positive electrode current collector. Even when an unexpected situation such as a short circuit occurs, the temporal and spatial concentration of heat generation due to the chemical reaction between the positive electrode active and the non-aqueous electrolyte is prevented.
【００１２】[0012]
【発明の実施の形態】以下、本発明に係る非水電解質電
池について、図面を参照しながら詳細に説明する。本発
明を適用した非水電解質二次電池はいわゆるリチウムイ
オン二次電池であり、正極活物質及び結着剤を含有する
正極活物質層が正極集電体上に複数積層されている正極
と、負極活物質及び結着剤を含有する負極活物質層が負
極集電体上に形成されている負極と、非水電解質として
液状の非水電解液とを備える。DETAILED DESCRIPTION OF THE PREFERRED EMBODIMENTS Hereinafter, a non-aqueous electrolyte battery according to the present invention will be described in detail with reference to the drawings. A nonaqueous electrolyte secondary battery to which the present invention is applied is a so-called lithium ion secondary battery, and a positive electrode in which a plurality of positive electrode active material layers containing a positive electrode active material and a binder are stacked on a positive electrode current collector, A negative electrode in which a negative electrode active material layer containing a negative electrode active material and a binder is formed on a negative electrode current collector, and a liquid nonaqueous electrolyte as a nonaqueous electrolyte.
【００１３】そして、この正極は、図１に示すように、
正極集電体１上に正極活物質層２が形成されており、正
極集電体１上に隣接する正極活物質層（以下、正極活物
質下層２ａと称する。）と、正極集電体１に隣接しない
正極活物質層、即ち、正極活物質下層２ａ上に形成され
る正極活物質層（以下、正極活物質上層２ｂと称す
る。）とを備える。また、正極活物質層２に含有される
正極活物質の組成は、その厚み方向において異なる。つ
まり、正極活物質下層２ａに含有される正極活物質と、
正極活物質上層２ｂに含有される正極活物質とは、組成
が異なる物質である。The positive electrode is, as shown in FIG.
A positive electrode active material layer 2 is formed on a positive electrode current collector 1, and a positive electrode active material layer adjacent to the positive electrode current collector 1 (hereinafter, referred to as a positive electrode active material lower layer 2 a) and a positive electrode current collector 1 are provided. , A positive electrode active material layer (hereinafter, referred to as a positive electrode active material upper layer 2b) formed on the positive electrode active material lower layer 2a. The composition of the positive electrode active material contained in the positive electrode active material layer 2 differs in the thickness direction. That is, the cathode active material contained in the cathode active material lower layer 2a,
The positive electrode active material contained in the positive electrode active material upper layer 2b is a material having a different composition.
【００１４】一般に、リチウムイオン二次電池の電池内
部でショートが発生した場合、ショート電流によりジュ
ール熱が発生する。このジュール熱は、熱の良導体であ
る正極集電体を通じて電池内部に拡散し、更に正極集電
体から正極活物質層中に拡散して正極活物質を加熱す
る。そして、ジュール熱により加熱された正極活物質は
非水電解質と化学反応を起こすため、この化学反応に起
因する高温の発熱が電池内部で生じることがある。Generally, when a short circuit occurs in a lithium ion secondary battery, Joule heat is generated due to the short current. This Joule heat diffuses into the battery through the positive electrode current collector, which is a good heat conductor, and further diffuses from the positive electrode current collector into the positive electrode active material layer to heat the positive electrode active material. Since the positive electrode active material heated by Joule heat causes a chemical reaction with the nonaqueous electrolyte, high-temperature heat generated by the chemical reaction may be generated inside the battery.
【００１５】ところで、正極活物質は、その組成が異な
ると非水電解質と化学反応を起こす温度も異なることが
知られている。つまり、この非水電解質二次電池におい
て、正極活物質下層２ａ及び正極活物質上層２ｂは、含
有する正極活物質の組成が異なるので、非水電解質と化
学反応を生じる温度が異なる。By the way, it is known that, when the composition of the positive electrode active material is different, the temperature at which a chemical reaction occurs with the nonaqueous electrolyte is also different. That is, in this non-aqueous electrolyte secondary battery, the positive electrode active material lower layer 2a and the positive electrode active material upper layer 2b have different compositions of the positive electrode active material, and therefore have different temperatures at which a chemical reaction occurs with the non-aqueous electrolyte.
【００１６】従って、この非水電解質二次電池は、電池
内部でショート等が発生して正極が加熱されたとして
も、正極活物質と非水電解質との化学反応による発熱の
時間的及び空間的な集中を防止されている。Therefore, in this non-aqueous electrolyte secondary battery, even if a short-circuit or the like occurs inside the battery and the positive electrode is heated, the time and space of heat generation due to the chemical reaction between the positive electrode active material and the non-aqueous electrolyte are increased. Concentration is prevented.
【００１７】この正極活物質層２は２層以上、４層以下
であることが好ましい。言い換えると、正極活物質上層
２ｂは１層以上、３層以下であることが好ましい。正極
活物質層２が４層を越える場合、電極を作製する製造コ
ストが高く付く可能性がある。The number of the positive electrode active material layers 2 is preferably two or more and four or less. In other words, it is preferable that the number of the positive electrode active material upper layer 2b is one or more and three or less. When the number of the positive electrode active material layers 2 exceeds four, there is a possibility that the manufacturing cost for manufacturing the electrode is increased.
【００１８】また、正極活物質下層２ａ及び正極活物質
上層２ｂの厚みとしては、正極活物質下層２ａの厚みを
１としたときに、正極活物質上層２ｂの厚みは０．１〜
２０の比率とすることが好ましい。The thickness of the positive electrode active material lower layer 2a and the thickness of the positive electrode active material upper layer 2b is 0.1 to 0.1 when the thickness of the positive electrode active material lower layer 2a is 1.
Preferably, the ratio is 20.
【００１９】正極活物質としては、一般式ＬｉxＭＯ
2（式中、０．０５≦ｘ≦１．１０範囲であり、Ｍは各
種遷移金属元素のうち、少なくとも１種類以上であ
る。）で表されるリチウム複合酸化物等の使用が可能で
ある。As the positive electrode active material, a general formula Li x MO
2 (wherein, in the range of 0.05 ≦ x ≦ 1.10, and M is at least one of various transition metal elements), etc., can be used. .
【００２０】正極活物質下層２ａが含有する正極活物質
としては、Ｍｎ又はＦｅのうち少なくとも１種類以上を
含有するＬｉ含有遷移金属酸化物であることが好まし
く、具体的にはＬｉＭｎ2Ｏ4、ＬｉＦｅＰＯ4、ＬｉＦ
ｅ1-xＭＰＯ4（式中、０＜ｘ≦１であり、ＭはＣｏ、Ｎ
ｉ、Ｍｎのうち何れか１種類以上である。）で表される
化合物のうち何れか１つ以上を含有することが好まし
い。The cathode active material contained in the cathode active material lower layer 2a is preferably a Li-containing transition metal oxide containing at least one of Mn and Fe, specifically, LiMn 2 O 4 , LiFePO 4 , LiF
e 1-x MPO 4 (where 0 <x ≦ 1 and M is Co, N
At least one of i and Mn. It is preferable to contain any one or more of the compounds represented by the formula (1).
【００２１】また、正極活物質上層２ｂが含有する正極
活物質としては、Ｎｉ又はＣｏのうち少なくとも１種類
以上を含有するＬｉ含有遷移金属酸化物であることが好
ましく、具体的にはＬｉＣｏＯ2、ＬｉＮｉＯ2、ＬｉＮ
ｉxＣｏ1-xＯ2、ＬｉＮｉxＣｏ1-x-yＡｌyＯ2（式中、
０＜ｘ＜１、０＜ｙ＜１である。）で表される化合物の
うち何れか１つ以上を含有することが好ましい。The cathode active material contained in the cathode active material upper layer 2b is preferably a Li-containing transition metal oxide containing at least one of Ni and Co, and specifically, LiCoO 2 , LiNiO 2 , LiN
i x Co 1-x O 2 , LiNi x Co 1-xy Al y O 2 ( wherein,
0 <x <1, 0 <y <1. It is preferable to contain any one or more of the compounds represented by the formula (1).
【００２２】正極活物質層２に含有される結着剤として
は、この種の電池の結着剤として従来より公知である樹
脂が何れも使用可能である。また、正極活物質層２に
は、従来より公知である導電材や種々添加剤等を含有さ
せても良い。As the binder contained in the positive electrode active material layer 2, any resin conventionally known as a binder for this type of battery can be used. The positive electrode active material layer 2 may contain a conventionally known conductive material, various additives, and the like.
【００２３】負極は、負極集電体上に、Ｌｉのドープ／
脱ドープが可能である負極活物質及び結着剤を含有する
負極合剤を塗布してなる負極活物質層が形成されてい
る。負極集電体としては、例えば銅箔等が用いられる。The negative electrode is formed by adding Li-doped /
A negative electrode active material layer formed by applying a negative electrode mixture containing a undoped negative electrode active material and a binder is formed. As the negative electrode current collector, for example, a copper foil or the like is used.
【００２４】負極活物質としては、Ｌｉのドープ／脱ド
ープが可能な炭素材料、難黒鉛化炭素系材料やグラファ
イト系材料等の炭素材料が使用可能である。より具体的
な炭素材料としては、熱分解炭素類、コークス類、（ピ
ッチコークス、ニードルコークス、石油コークス等）、
グラファイト類、ガラス状炭素類、有機高分子化合物焼
成体（フェノール樹脂、フラン樹脂等を適当な温度で焼
成し炭素化したもの。）、炭素繊維、活性炭等が使用可
能である。As the negative electrode active material, a carbon material capable of doping / dedoping Li, a non-graphitizable carbon-based material and a graphite-based material can be used. More specific carbon materials include pyrolytic carbons, cokes, (pitch coke, needle coke, petroleum coke, etc.),
Graphites, glassy carbons, organic polymer compound fired bodies (phenol resins, furan resins, etc. fired at an appropriate temperature and carbonized), carbon fibers, activated carbon, and the like can be used.
【００２５】負極合剤を調製する際に負極活物質と混合
する結着剤としては、この種の電池の結着剤として従来
より公知である樹脂が何れも使用可能である。As the binder to be mixed with the negative electrode active material when preparing the negative electrode mixture, any resin conventionally known as a binder for this type of battery can be used.
【００２６】非水電解質は、非水溶媒に電解質塩を溶解
して調製される液状のいわゆる電解液である。The non-aqueous electrolyte is a so-called liquid electrolyte prepared by dissolving an electrolyte salt in a non-aqueous solvent.
【００２７】非水溶媒としては、炭酸プロピレン、炭酸
エチレン等の環状炭酸エステルや、炭酸ジメチル、炭酸
ジエチル等の鎖状炭酸エステルや、プロピオン酸メチ
ル、酪酸メチル等のカルボン酸エステル、γ−ブチロラ
クトン、スルホラン、２−メチルテトラヒドロフラン、
ジメトキシエタン等のエーテル類が使用可能である。酸
化安定性の点からは、特に炭酸エステルを含有させるこ
とが好ましい。また、これらの非水溶媒は、１種類を単
独で用いても良いし、２種類以上を混合して用いても良
い。Examples of the non-aqueous solvent include cyclic carbonates such as propylene carbonate and ethylene carbonate, chain carbonates such as dimethyl carbonate and diethyl carbonate, carboxylate esters such as methyl propionate and methyl butyrate, γ-butyrolactone, Sulfolane, 2-methyltetrahydrofuran,
Ethers such as dimethoxyethane can be used. From the viewpoint of oxidation stability, it is particularly preferable to include a carbonate ester. One of these nonaqueous solvents may be used alone, or two or more of them may be used in combination.
【００２８】電解質塩としては、例えばＬｉＰＦ6、Ｌ
ｉＢＦ4、ＬｉＡｓＦ6、ＬｉＣｌＯ4、ＬｉＣＦ3Ｓ
Ｏ3、ＬｉＮ（ＳＯ2ＣＦ3）2、ＬｉＣ（ＳＯ2Ｃ
Ｆ3）3、ＬｉＡｌＣｌ4、ＬｉＳｉＦ6等のリチウム塩が
使用可能である。酸化に対する安定性の点からは、特に
これらのリチウム塩の中でもＬｉＰＦ6、ＬｉＢＦ4を使
用することが好ましい。これら電解質塩を非水溶媒に溶
解する濃度は、０．１ｍｏｌ／ｌ以上、５．０ｍｏｌ／
ｌ以下の範囲であることが好ましく、０．５ｍｏｌ／ｌ
以上、３．０ｍｏｌ／ｌ以下の範囲であることがより好
ましい。また、非水溶媒には、フッ素系高分子化合物を
添加してもよい。As the electrolyte salt, for example, LiPF 6 , L
iBF 4 , LiAsF 6 , LiClO 4 , LiCF 3 S
O 3 , LiN (SO 2 CF 3 ) 2 , LiC (SO 2 C
Lithium salts such as F 3 ) 3 , LiAlCl 4 and LiSiF 6 can be used. From the viewpoint of stability against oxidation, it is particularly preferable to use LiPF 6 or LiBF 4 among these lithium salts. The concentration at which these electrolyte salts are dissolved in the non-aqueous solvent is 0.1 mol / l or more and 5.0 mol / l.
1 mol or less, preferably 0.5 mol / l
More preferably, the range is 3.0 mol / l or less. In addition, a fluorine-based polymer compound may be added to the non-aqueous solvent.
【００２９】この非水電解質二次電池は、例えば図２に
示すように、正極集電体１上に正極活物質を含有する正
極活物質層２が複数積層されている帯状の正極３と、負
極集電体４上に負極活物質を含有する負極活物質層が形
成されている帯状の負極５とがセパレータ６を介して積
層され、長手方向に巻回されてなる渦巻型の電極体が電
池缶７に装填され、非水電解質として液状の非水電解液
が電池缶７に注入されている。そして、電池蓋８が、絶
縁封口ガスケット９を介して電池缶７とかしめて固定さ
れている。また、この非水電解質二次電池は、負極リー
ド１０および正極リード１１に接続するセンターピン１
２が設けられているとともに、電池内部の圧力が所定値
よりも高くなったときに内部の気体を抜くための安全弁
装置１３及び電池内部の温度上昇を防止するためのＰＴ
Ｃ素子１４が設けられている。なお、本発明を適用した
非水電解質二次電池の形状は、角形、コイン型、ボタン
型、シート型等の何れであっても良く、またその大きさ
も限定されない。The non-aqueous electrolyte secondary battery includes, as shown in FIG. 2, for example, a strip-shaped positive electrode 3 in which a plurality of positive electrode active material layers 2 containing a positive electrode active material are laminated on a positive electrode current collector 1; A strip-shaped negative electrode 5 in which a negative electrode active material layer containing a negative electrode active material is formed on a negative electrode current collector 4 is laminated with a separator 6 interposed therebetween, and a spiral electrode body formed by being wound in the longitudinal direction is formed. A liquid non-aqueous electrolyte is charged into the battery can 7 as a non-aqueous electrolyte. Then, the battery cover 8 is fixed by caulking to the battery can 7 via the insulating sealing gasket 9. The nonaqueous electrolyte secondary battery has a center pin 1 connected to a negative electrode lead 10 and a positive electrode lead 11.
2 and a safety valve device 13 for releasing gas inside the battery when the pressure inside the battery becomes higher than a predetermined value, and a PT for preventing a rise in temperature inside the battery.
A C element 14 is provided. The shape of the non-aqueous electrolyte secondary battery to which the present invention is applied may be any of a square shape, a coin shape, a button shape, a sheet shape, and the like, and the size is not limited.
【００３０】以上のように構成された非水電解液二次電
池は、電極が変形をするような異常な状況下で使用され
て、ショートが生じるといった不測の事態に陥った場合
でも、安定性に優れる。The non-aqueous electrolyte secondary battery constructed as described above is used under an abnormal situation where the electrode is deformed, and even when an unexpected situation such as a short circuit occurs, the stability is maintained. Excellent.
【００３１】[0031]
【実施例】以下、本発明について、具体的な実験結果に
基づいて詳細に説明する。発明の主旨を越えない限り、
本発明は実施例に限定されるものではない。DESCRIPTION OF THE PREFERRED EMBODIMENTS The present invention will be described below in detail based on specific experimental results. Unless it goes beyond the gist of the invention,
The present invention is not limited to the embodiments.
【００３２】〔正極の作製〕先ず、正極活物質の組成が
異なる正極合剤を複数調製した。[Preparation of Positive Electrode] First, a plurality of positive electrode mixtures having different compositions of the positive electrode active material were prepared.
【００３３】正極合剤Ａ 正極活物質としてＬｉＮｉＯ2を９１重量部、導電材と
してグラファイトを６重量部、及び結着剤としてポリフ
ッ化ビニリデンを３重量部を混合して正極合剤Ａを調製
した。そして、これをＮ−メチル−２−ピロリドン中に
分散させてスラリー状の正極合剤Ａとした。 Positive electrode mixture A 91 parts by weight of LiNiO 2 as a positive electrode active material, 6 parts by weight of graphite as a conductive material, and 3 parts by weight of polyvinylidene fluoride as a binder were mixed to prepare a positive electrode mixture A. . Then, this was dispersed in N-methyl-2-pyrrolidone to obtain a positive electrode mixture A in a slurry state.
【００３４】正極合剤Ｂ 正極活物質としてＬｉＣｏＯ2を混合したこと以外は正
極合剤Ａと同様にして、正極合剤Ｂを調製した。 Positive electrode mixture B A positive electrode mixture B was prepared in the same manner as the positive electrode mixture A except that LiCoO 2 was mixed as the positive electrode active material.
【００３５】正極合剤Ｃ 正極活物質としてＬｉＮｉ0.8Ｃｏ0.2Ｏ2を混合したこ
と以外は正極合剤Ａと同様にして、正極合剤Ｃを調製し
た。 Positive electrode mixture C A positive electrode mixture C was prepared in the same manner as the positive electrode mixture A except that LiNi 0.8 Co 0.2 O 2 was mixed as the positive electrode active material.
【００３６】正極合剤Ｄ 正極活物質としてＬｉＭｎ2Ｏ4を混合したこと以外は正
極合剤Ａと同様にして、正極合剤Ｄを調製した。Positive electrode mixture D A positive electrode mixture D was prepared in the same manner as the positive electrode mixture A except that LiMn 2 O 4 was mixed as the positive electrode active material.
【００３７】正極合剤Ｅ 正極活物質としてＬｉＦｅＰＯ4を混合したこと以外は
正極合剤Ａと同様にして、正極合剤Ｅを調製した。Positive electrode mixture E A positive electrode mixture E was prepared in the same manner as the positive electrode mixture A except that LiFePO 4 was mixed as a positive electrode active material.
【００３８】正極合剤Ｆ 正極活物質としてＬｉＮｉＯ2を４５重量部と、ＬｉＭ
ｎ2Ｏ4を４６重量部とを混合したこと以外は正極合剤Ａ
と同様にして、正極合剤Ｆを調製した。Positive electrode mixture F : 45 parts by weight of LiNiO 2 as a positive electrode active material;
positive electrode mixture A except that n 2 O 4 was mixed with 46 parts by weight.
In the same manner as in the above, a positive electrode mixture F was prepared.
【００３９】次に、上述のように調製したスラリー状の
各種正極合剤を表１に示す組み合わせ及び塗布厚みとし
て、正極集電体上となる厚さが２０μｍである帯状のア
ルミニウム箔の両面に正極活物質層を形成した。Next, the various positive electrode mixtures in the form of slurry prepared as described above were used as combinations and coating thicknesses shown in Table 1 on both sides of a strip-shaped aluminum foil having a thickness of 20 μm on the positive electrode current collector. A positive electrode active material layer was formed.
【００４０】[0040]
【表１】 [Table 1]
【００４１】実施例１〜実施例６の正極は以下に示すよ
うにして作製した。まず、正極活物質下層を形成する正
極合剤を正極集電体の両面に均一に塗布して乾燥させ
た。次に、乾燥させた正極活物質下層上に、正極活物質
上層を形成する正極合剤を均一に塗布して乾燥させた。
そして、ロールプレス機を用いて圧縮成型した後にスリ
ットすることで、帯状の正極を得た。比較例１〜比較例
４の正極は、上記表１に示す正極合剤を正極集電体の両
面に均一に塗布して乾燥させ、一定圧力で圧縮成型した
後にスリットすることで、帯状の正極を得た。なお、正
極活物質下層及び正極活物質上層の塗布厚みは、各正極
を圧縮成形した後に、正極の断面を電子顕微鏡を用いて
測定した。The positive electrodes of Examples 1 to 6 were produced as described below. First, the positive electrode mixture forming the lower layer of the positive electrode active material was uniformly applied on both surfaces of the positive electrode current collector and dried. Next, the positive electrode mixture forming the positive electrode active material upper layer was uniformly applied on the dried positive electrode active material lower layer, and dried.
Then, a band-shaped positive electrode was obtained by slitting after compression molding using a roll press machine. The positive electrodes of Comparative Examples 1 to 4 were uniformly coated with the positive electrode mixture shown in Table 1 above on both sides of the positive electrode current collector, dried, compression-molded at a constant pressure, and then slit. I got In addition, the coating thickness of the lower layer of the positive electrode active material and the upper layer of the positive electrode active material was measured using an electron microscope on the cross section of each positive electrode after compression molding of each positive electrode.
【００４２】〔負極の作製〕負極活物質として人造黒鉛
（ロンザ社製 商品名：ＫＳ−６）を９６重量部と、結
着剤としてスチレンブタジエンゴムを３重量部及びカル
ボキシメチルセルロースを１重量部とを水中で混合し
て、スラリー状の負極合剤を調製した。[Preparation of Negative Electrode] 96 parts by weight of artificial graphite (trade name: KS-6, manufactured by Lonza) as a negative electrode active material, 3 parts by weight of styrene butadiene rubber and 1 part by weight of carboxymethyl cellulose as a binder. Was mixed in water to prepare a slurry-like negative electrode mixture.
【００４３】そして、負極集電体となる厚さが１０μｍ
である帯状の銅箔の両面に、スラリー状の負極合剤を均
一に塗布して乾燥させ、ロールプレス機を用いて圧縮成
型した後にスリットすることで、帯状の負極を作製し
た。The thickness of the negative electrode current collector is 10 μm.
A slurry-like negative electrode mixture was uniformly applied to both sides of the strip-shaped copper foil, dried, compression-molded using a roll press, and then slit to produce a strip-shaped negative electrode.
【００４４】〔非水電解液の調製〕非水溶媒として炭酸
エチレンを４０容量％と炭酸メチルエチルを６０容量％
として混合した混合溶媒中に、電解質塩としてＬｉＰＦ
6を１．０ｍｏｌ／ｌの割合で溶解させて非水電解液を
調製した。[Preparation of Nonaqueous Electrolyte] As a nonaqueous solvent, 40% by volume of ethylene carbonate and 60% by volume of methyl ethyl carbonate were used.
LiPF as an electrolyte salt in a mixed solvent mixed as
6 was dissolved at a rate of 1.0 mol / l to prepare a non-aqueous electrolyte.
【００４５】〔非水電解液二次電池の作製〕上述のよう
にして作製した実施例１〜実施例６及び比較例１〜比較
例４の帯状の正極と帯状の負極とを、厚さが２５μｍで
あり微孔性ポリプロピレンフィルムからなるセパレータ
を介して、負極、セパレータ、正極、セパレータの順に
積層した後に多数回巻き回して、渦巻型の電極体を複数
作製した。[Preparation of Nonaqueous Electrolyte Secondary Battery] The band-shaped positive electrode and the band-shaped negative electrode of Examples 1 to 6 and Comparative Examples 1 to 4 prepared as described above were A negative electrode, a separator, a positive electrode, and a separator were laminated in this order via a separator made of a microporous polypropylene film having a thickness of 25 μm, and then wound many times to produce a plurality of spiral electrode bodies.
【００４６】次に、ニッケルメッキを施した鉄製の電池
缶に、絶縁板を底部に挿入した後に、この電極体を収納
した。そして、負極の集電をとるために、ニッケル製の
負極リードの一端を負極に圧着し、他端を電池缶に溶接
した。また、正極の集電をとるために、アルミニウム製
の正極リードの一端を正極に圧着し、他端を電池内圧に
応じて電流を遮断する電流遮断用薄板を介して電池蓋に
溶接した。そして、電池缶の中に上述のようにして調製
した非水電解液を注入した後に、アスファルトを塗布し
た絶縁封口ガスケットを介して電池缶をかしめることに
より電池蓋を固定することで、円筒型であり、直径が１
８ｍｍ、高さが６５ｍｍである実施例１〜実施例６及び
比較例１〜比較例４の非水電解液二次電池を作製した。Next, after inserting the insulating plate into the bottom of the nickel-plated iron battery can, the electrode body was housed. Then, in order to collect the current of the negative electrode, one end of a nickel negative electrode lead was pressed against the negative electrode, and the other end was welded to the battery can. Further, in order to collect the current of the positive electrode, one end of an aluminum positive electrode lead was crimped to the positive electrode, and the other end was welded to the battery lid via a current interrupting thin plate for interrupting current according to the internal pressure of the battery. Then, after injecting the non-aqueous electrolyte prepared as described above into the battery can, the battery can is caulked through an insulating sealing gasket coated with asphalt to fix the battery lid, thereby obtaining a cylindrical battery. And has a diameter of 1
Non-aqueous electrolyte secondary batteries of Examples 1 to 6 and Comparative Examples 1 to 4 having a height of 8 mm and a height of 65 mm were produced.
【００４７】以上のようにして作製した非水電解液二次
電池に対して、はじめに、充電電流を１．０Ａとし、終
止電圧を４．２Ｖとして定電流定電圧充電を３時間行っ
た。そして、これら電池の放電特性を評価するために、
放電電流を７００ｍＡとし、終止電圧を２．５Ｖとして
定電流放電を行って初期容量を測定した。The non-aqueous electrolyte secondary battery produced as described above was first charged at a constant current of 1.0 A and a constant voltage of 4.2 V for three hours at a constant current and a constant voltage. And, in order to evaluate the discharge characteristics of these batteries,
A constant current discharge was performed at a discharge current of 700 mA and a final voltage of 2.5 V, and the initial capacity was measured.
【００４８】次に、電池内部でショートが生じた場合に
おけるこれら電池の安定性を評価するために、充電電流
を１．０Ａとし、終止電圧を４．４Ｖとして定電流定電
圧充電を３時間行った後、直径が５ｍｍである鉄釘を、
プレス機を用いて、電池中央に貫通するまで刺し、電池
内部でショートを生じさせた。この時、電池缶壁の温度
変化を観察し、その最高温度を測定した。なお、何れの
電池においてもガス噴出や破裂等は発生せず、電池缶内
に充填されている種々の充填物は電池缶外に流出してい
ない。また、これら一連の測定は、２３℃環境下におい
て行った。Next, in order to evaluate the stability of these batteries when a short circuit occurs inside the batteries, the charging current was set to 1.0 A, the final voltage was set to 4.4 V, and the constant current and constant voltage charging was performed for 3 hours. After that, an iron nail with a diameter of 5 mm
Using a press machine, the battery was stabbed until it penetrated the center of the battery, thereby causing a short circuit inside the battery. At this time, the temperature change of the battery can wall was observed, and the maximum temperature was measured. In addition, in any of the batteries, no gas ejection or rupture occurred, and the various fillers filled in the battery can did not flow out of the battery can. These series of measurements were performed in a 23 ° C. environment.
【００４９】以上のようにして測定した実施例１〜実施
例８及び比較例１〜比較例８の非水電解液二次電池の初
期容量、及び電極ショート時の最高温度を表２に示す。Table 2 shows the initial capacities of the nonaqueous electrolyte secondary batteries of Examples 1 to 8 and Comparative Examples 1 to 8 measured as described above, and the maximum temperature at the time of electrode short-circuit.
【００５０】[0050]
【表２】 [Table 2]
【００５１】表２から明らかなように、正極活物質層が
正極集電体上に複数積層され、かつ、正極活物質層に含
有される正極活物質の組成がその厚み方向において異な
る正極を備える実施例１〜実施例６の非水電解液二次電
池は、電極ショートにより電極が発熱した場合でも発生
した熱が電池内部で拡散されるので、電極ショート時の
最高温度は９０℃以下であり、温度上昇が抑制されてい
ることがわかった。As is clear from Table 2, a plurality of positive electrode active material layers are stacked on the positive electrode current collector, and a positive electrode in which the composition of the positive electrode active material contained in the positive electrode active material layer differs in the thickness direction is provided. In the non-aqueous electrolyte secondary batteries of Examples 1 to 6, since the generated heat is diffused inside the battery even when the electrode generates heat due to the electrode short, the maximum temperature at the time of electrode short is 90 ° C. or less. It was found that the temperature rise was suppressed.
【００５２】これに対して、正極活物質層が単層である
正極を備える比較例１から比較例４の非水電解液二次電
池は、電極ショート時の最高温度は１００℃を越えてし
まうことがわかった。On the other hand, in the nonaqueous electrolyte secondary batteries of Comparative Examples 1 to 4 including the positive electrode in which the positive electrode active material layer is a single layer, the maximum temperature at the time of electrode short-circuit exceeds 100 ° C. I understand.
【００５３】また、実施例１〜実施例６の非水電解液二
次電池は、比較例１〜比較例４の非水電解液二次電池と
比較すると、正極活物質層が正極集電体上に複数積層さ
れている正極をを備えていても電池の初期容量は同等で
あり、所望の放電特性を満たしていることがわかった。The non-aqueous electrolyte secondary batteries of Examples 1 to 6 have a positive electrode active material layer having a positive electrode current collector when compared with the non-aqueous electrolyte secondary batteries of Comparative Examples 1 to 4. It was found that the batteries had the same initial capacity even when a plurality of positive electrodes were stacked thereon, and thus satisfied the desired discharge characteristics.
【００５４】従って、非水電解液二次電池は、正極活物
質層が正極集電体上に複数積層され、かつ、正極活物質
層に含有される正極活物質の組成がその厚み方向におい
て異なる正極を備えることにより、安定性に優れること
がわかった。Therefore, in the nonaqueous electrolyte secondary battery, a plurality of positive electrode active material layers are laminated on the positive electrode current collector, and the composition of the positive electrode active material contained in the positive electrode active material layer differs in the thickness direction. It was found that the provision of the positive electrode was excellent in stability.
【００５５】[0055]
【発明の効果】以上の説明からも明らかなように、非水
電解質電池は、正極活物質層が正極集電体上に複数積層
され、かつ、正極活物質層に含有される正極活物質の組
成がその厚み方向において異なる正極を備えることによ
り、電極が変形するような異常な状況下で使用され、シ
ョートが生じるといった不測の事態に陥った場合でも、
安定性に優れる。As is apparent from the above description, in the nonaqueous electrolyte battery, a plurality of positive electrode active material layers are stacked on the positive electrode current collector, and the positive electrode active material layer contained in the positive electrode active material layer is By providing a positive electrode whose composition is different in its thickness direction, it is used under abnormal conditions such as deformation of the electrode, even if an unexpected situation such as short circuit occurs,
Excellent stability.
【図１】本発明を適用した非水電解質二次電池が備える
正極の要部断面図である。FIG. 1 is a sectional view of a main part of a positive electrode provided in a nonaqueous electrolyte secondary battery to which the present invention is applied.
【図２】非水電解液二次電池の一構成例を示す断面図で
ある。FIG. 2 is a cross-sectional view illustrating a configuration example of a non-aqueous electrolyte secondary battery.
【符号の説明】 １ 正極集電体、２ 正極活物質層、２ａ 正極活物質
下層、２ｂ 正極活物質上層[Description of Signs] 1 positive electrode current collector, 2 positive electrode active material layer, 2a lower layer of positive electrode active material, 2b upper layer of positive electrode active material
Claims (6)
極集電体上に複数積層されている正極と、 負極活物質を含有する負極と、 非水電解質とを備え、 当該正極活物質層に含有される当該正極活物質の組成
は、その厚み方向において異なることを特徴とする非水
電解質電池。1. A positive electrode comprising a positive electrode in which a plurality of positive electrode active material layers containing a positive electrode active material are laminated on a positive electrode current collector, a negative electrode containing a negative electrode active material, and a non-aqueous electrolyte. A non-aqueous electrolyte battery, wherein the composition of the positive electrode active material contained in the layer differs in the thickness direction.
を正極活物質下層とするとき、当該正極活物質下層が含
有する正極活物質は、Ｍｎ又はＦｅのうち少なくとも１
種類以上を含有するＬｉ含有遷移金属酸化物を含有する
ことを特徴とする請求項１記載の非水電解質電池。2. When the cathode active material layer adjacent to the cathode current collector is used as a cathode active material lower layer, the cathode active material contained in the cathode active material lower layer contains at least one of Mn and Fe.
The non-aqueous electrolyte battery according to claim 1, further comprising a Li-containing transition metal oxide containing at least one kind.
層を正極活物質上層とするとき、当該正極活物質上層が
含有する正極活物質は、Ｎｉ又はＣｏのうち少なくとも
１種類以上を含有するＬｉ含有遷移金属酸化物であるこ
とを特徴とする請求項１記載の非水電解質電池。3. When a positive electrode active material layer not adjacent to the positive electrode current collector is used as a positive electrode active material upper layer, the positive electrode active material contained in the positive electrode active material upper layer contains at least one kind of Ni or Co. The non-aqueous electrolyte battery according to claim 1, which is a Li-containing transition metal oxide.
を特徴とする請求項１記載の非水電解質電池。4. The non-aqueous electrolyte battery according to claim 1, wherein the negative electrode active material is a carbon material.
質は、ＬｉＭｎ2Ｏ4、ＬｉＦｅＰＯ4、ＬｉＦｅ1-xＭＰ
Ｏ4（式中、０＜ｘ≦１であり、ＭはＣｏ、Ｎｉ、Ｍｎ
のうち何れか１種類以上である。）で表される化合物の
うち何れか１つ以上を含有することを特徴とする請求項
２記載の非水電解質電池。5. The positive electrode active material contained in the lower layer of the positive electrode active material includes LiMn 2 O 4 , LiFePO 4 , and LiFe 1-x MP.
O 4 (where 0 <x ≦ 1, and M is Co, Ni, Mn
At least one of them. 3. The non-aqueous electrolyte battery according to claim 2, wherein the non-aqueous electrolyte battery contains at least one compound selected from the group consisting of:
質は、ＬｉＣｏＯ2、ＬｉＮｉＯ2、ＬｉＮｉxＣｏ1-xＯ
2、ＬｉＮｉxＣｏ1-x-yＡｌyＯ2（式中、０＜ｘ＜１、
０＜ｙ＜１である。）で表される化合物のうち何れか１
つ以上を含有することを特徴とする請求項３記載の非水
電解質電池。6. The positive electrode active material contained in the upper layer of the positive electrode active material is LiCoO 2 , LiNiO 2 , LiNi x Co 1-x O
2 , LiNi x Co 1-xy Al y O 2 (where 0 <x <1,
0 <y <1. Any one of the compounds represented by
4. The non-aqueous electrolyte battery according to claim 3, comprising at least one.
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