JPH06150971A - Cylindrical nonaqueous electrolyte secondary battery - Google Patents
Cylindrical nonaqueous electrolyte secondary batteryInfo
- Publication number
- JPH06150971A JPH06150971A JP4292880A JP29288092A JPH06150971A JP H06150971 A JPH06150971 A JP H06150971A JP 4292880 A JP4292880 A JP 4292880A JP 29288092 A JP29288092 A JP 29288092A JP H06150971 A JPH06150971 A JP H06150971A
- Authority
- JP
- Japan
- Prior art keywords
- electrode
- battery
- adhesive tape
- aqueous electrolyte
- secondary 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
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Landscapes
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Secondary Cells (AREA)
Abstract
Description
【0001】[0001]
【産業上の利用分野】本発明は、電極と帯状セパレータ
とを積層後、渦巻状に巻回した渦巻式電極を電池缶内に
挿入する円筒型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 relates to a cylindrical non-aqueous electrolyte secondary battery in which an electrode and a strip separator are laminated and a spirally wound electrode is inserted into a battery can.
【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、移動用電源としての電池に対しても益々小型・軽
量且つ高エネルギ密度のものが求められている。2. Description of the Related Art Recent remarkable advances in electronic technology have made electronic devices smaller and lighter one after another. Along with this, there is an increasing demand for batteries as mobile power sources that are smaller, lighter, and have higher energy density.
【0003】従来、一般用途の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。これらの電池はサイクル特性には優れるが、
電池重量やルネルギ密度の点では十分満足できる特性と
は言えない。Conventionally, an aqueous solution type battery such as a lead battery or a nickel-cadmium battery has been mainly used as a secondary battery for general use. Although these batteries have excellent cycle characteristics,
It cannot be said that the characteristics are sufficiently satisfactory in terms of battery weight and Lunergi density.
【0004】最近、リチウム或はリチウム合金を負極に
用いた非水電解液二次電池の研究・開発が盛んに行われ
ている。この電池は高エネルギ密度を有し、自己放電も
少なく、軽量という優れた特性を有するが、充放電サイ
クルの進行に伴い、充電時にリチウムがデンドライト状
に結晶成長し、正極に到達して内部ショートに至る可能
性が高くなる欠点があり、実用化への大きな障害となっ
ている。Recently, non-aqueous electrolyte secondary batteries using lithium or a lithium alloy as a negative electrode have been actively researched and developed. This battery has high energy density, low self-discharge, and excellent characteristics such as light weight, but as the charge / discharge cycle progresses, lithium grows into dendrite-like crystals during charging and reaches the positive electrode, causing an internal short circuit. There is a drawback that the possibility of reaching a high level is high, which is a major obstacle to practical use.
【0005】これに対し、負極に炭素材料を使用した非
水電解液二次電池は、化学的、物理的方法により、予め
炭素材料に担持させたリチウム、正極活物質の結晶構造
中のリチウム、電解液中に溶解しているリチウム等の、
炭素層間へのドープ/脱ドープを利用するもので、充放
電サイクルが進行しても充電時のデンドライト状の析出
が見られず、1000回を超える優れた充放電サイクル
特性を示す。On the other hand, the non-aqueous electrolyte secondary battery using a carbon material for the negative electrode has lithium preliminarily supported on the carbon material by chemical and physical methods, lithium in the crystal structure of the positive electrode active material, Such as lithium dissolved in the electrolyte,
It utilizes doping / dedoping between carbon layers, and does not show dendrite-like precipitation during charging even if the charging / discharging cycle progresses, and exhibits excellent charging / discharging cycle characteristics exceeding 1000 times.
【0006】これらの材料を用いた非水電解液二次電池
の用途としては、ビデオ・カメラやラップ・トップ・パ
ソコン等が挙げられるが、このような機器は比較的消費
電流が大きいものが多く、電池構造としては渦巻式電極
構造が有効である。これは、帯状正極と帯状負極とをセ
パレータを介して渦巻状に巻いたもので、電極面積が大
きくとれることから重負荷に耐えられる。Non-aqueous electrolyte secondary batteries using these materials include video cameras, laptops, personal computers, etc., but most of these devices have relatively large current consumption. The spiral electrode structure is effective as the battery structure. This is a spirally wound band-shaped positive electrode and band-shaped negative electrode with a separator interposed therebetween, and since a large electrode area can be obtained, a heavy load can be endured.
【0007】一方、電池特性は電極間に圧力が加わって
いる方が良い傾向がある。しかしながら、電池の組立工
程に於いてこのような電極を電池缶に挿入する際、生産
性の点から電極外径と電池缶内径との間にはある程度の
クリアランスを設ける必要がある。巻回した電極は最外
周巻き終わり部を粘着テープにより固定し、緩まないよ
うにする方法が一般的に採られる。本発明者は、特願平
2−317428に示すように、電極の幅方向に対す
る、粘着テープの幅方向占有率を規定することにより、
非水電解液二次電池の充放電サイクル特性が向上するこ
とを見だした。On the other hand, the battery characteristics tend to be better when pressure is applied between the electrodes. However, when inserting such an electrode into a battery can in the process of assembling a battery, it is necessary to provide some clearance between the outer diameter of the electrode and the inner diameter of the battery can from the viewpoint of productivity. In general, a method of fixing the outermost peripheral end of the wound electrode with an adhesive tape so that it does not loosen is adopted. As disclosed in Japanese Patent Application No. 2-317428, the present inventor defines the occupancy ratio of the adhesive tape in the width direction with respect to the width direction of the electrode.
It has been found that the charge / discharge cycle characteristics of the non-aqueous electrolyte secondary battery are improved.
【0008】[0008]
【発明が解決しようとする課題】しかしながら、この方
法を採用しても種々の変動要因によって、サイクル劣化
の不十分なロットが生じるという問題があった。そこ
で、より信頼性の高い非水電解液二次電池を生産するた
めに、さらにサイクル劣化を向上させる手法の開発が望
まれている。However, even if this method is adopted, there is a problem that lots with insufficient cycle deterioration occur due to various fluctuation factors. Therefore, in order to produce a more reliable non-aqueous electrolyte secondary battery, development of a method for further improving cycle deterioration is desired.
【0009】本発明はこのような課題に鑑みてなされた
ものであり、充放電サイクル特性の優れた円筒型非水電
解液二次電池を得ることを目的とする。The present invention has been made in view of the above problems, and an object thereof is to obtain a cylindrical non-aqueous electrolyte secondary battery having excellent charge / discharge cycle characteristics.
【0010】[0010]
【課題を解決するための手段】本発明の円筒型非水電解
液二次電池は、例えば図1に示すように、帯状負極及び
帯状正極をセパレータを介して積層するように渦巻状に
巻回し、その巻き終わり部を粘着テープ20を用いて固
定される渦巻式電極15を非水電解液とともに電池缶内
に収容してなる円筒型非水電解液二次電池において、こ
の渦巻式電極15の外径をLとし、巻き終わり部を固定
する粘着テープ20のこの外径に沿う長さをkπLとす
るとき、k≧0.6であるものである。A cylindrical non-aqueous electrolyte secondary battery of the present invention is, for example, as shown in FIG. 1, spirally wound so that a strip negative electrode and a strip positive electrode are laminated with a separator interposed therebetween. In a cylindrical non-aqueous electrolyte secondary battery in which a spirally wound electrode 15 whose end of winding is fixed with an adhesive tape 20 is housed in a battery can together with a non-aqueous electrolyte, the spirally wound electrode 15 When the outer diameter is L and the length along the outer diameter of the adhesive tape 20 for fixing the winding end portion is kπL, k ≧ 0.6.
【0011】また、本発明の円筒型非水電解液二次電池
は、例えば、図6に示すように、帯状負極及び帯状正極
をセパレータを介して積層するように渦巻状に巻回し、
その巻き終わり部を粘着テープ20を用いて固定される
渦巻式電極15を非水電解液とともに電池缶内に収容し
てなる円筒型非水電解液二次電池において、この粘着テ
ープ20は支持体上に粘着層を有してなり、この支持体
はこの電解液との接触により膨潤し、体積膨張する材料
よりなるものである。Further, the cylindrical non-aqueous electrolyte secondary battery of the present invention is, for example, as shown in FIG. 6, spirally wound so that a strip negative electrode and a strip positive electrode are laminated via a separator,
In a cylindrical non-aqueous electrolyte secondary battery in which a spirally wound electrode 15 whose end of winding is fixed using an adhesive tape 20 is housed in a battery can together with a non-aqueous electrolyte, the adhesive tape 20 is a support. The support has an adhesive layer on the top, and the support is made of a material that swells upon contact with the electrolytic solution and expands in volume.
【0012】また、本発明の円筒型非水電解液二次電池
は、帯状負極及び帯状正極をセパレータを介して積層す
るように渦巻状に巻回し、その巻き終わり部を粘着テー
プ20を用いて固定される渦巻式電極15を非水電解液
とともに電池缶内に収容してなる円筒型非水電解液二次
電池において、この渦巻式電極15の外径をLとし、巻
き終わり部を固定する粘着テープ20のこの外径に沿う
長さをkπLとするとき、k≧0.6であり、かつ、こ
の粘着テープ20は支持体上に粘着層を有してなり、こ
の支持体はこの電解液との接触により膨潤し、体積膨張
する材料よりなるものである。Further, in the cylindrical non-aqueous electrolyte secondary battery of the present invention, the strip-shaped negative electrode and the strip-shaped positive electrode are spirally wound so as to be laminated with the separator interposed therebetween, and the winding end portion is coated with the adhesive tape 20. In a cylindrical non-aqueous electrolyte secondary battery in which a fixed spiral electrode 15 is housed in a battery can together with a non-aqueous electrolyte, the outer diameter of the spiral electrode 15 is set to L, and the end of winding is fixed. When the length of the pressure-sensitive adhesive tape 20 along this outer diameter is kπL, k ≧ 0.6, and the pressure-sensitive adhesive tape 20 has a pressure-sensitive adhesive layer on a support. It is made of a material that swells upon contact with a liquid and expands in volume.
【0013】[0013]
【作用】本発明の円筒型非水電解液二次電池によれば、
帯状負極及び帯状正極をセパレータを介して積層するよ
うに渦巻状に巻回し、その巻き終わり部を粘着テープ2
0を用いて固定される渦巻式電極15を非水電解液とと
もに電池缶内に収容してなる円筒型非水電解液二次電池
において、この渦巻式電極15の外径をLとし、巻き終
わり部を固定する粘着テープ20のこの外径に沿う長さ
をkπLとするとき、k≧0.6であるものとすること
により、粘着テープの長さを規定するので、円筒型非水
電解液二次電池の充放電サイクル特性を向上させること
ができる。According to the cylindrical non-aqueous electrolyte secondary battery of the present invention,
The strip-shaped negative electrode and the strip-shaped positive electrode are spirally wound so as to be laminated via a separator, and the end of the winding is adhered to the adhesive tape 2
In a cylindrical non-aqueous electrolyte secondary battery in which a spirally wound electrode 15 fixed by using 0 is housed in a battery can together with a non-aqueous electrolyte, the outer diameter of the spirally wound electrode 15 is set to L, and winding ends. When the length of the pressure-sensitive adhesive tape 20 for fixing the parts along this outer diameter is kπL, the length of the pressure-sensitive adhesive tape is defined by setting k ≧ 0.6. Therefore, the cylindrical non-aqueous electrolyte solution is used. The charge / discharge cycle characteristics of the secondary battery can be improved.
【0014】また、本発明の円筒型非水電解液二次電池
によれば、帯状負極及び帯状正極をセパレータを介して
積層するように渦巻状に巻回し、その巻き終わり部を粘
着テープ20を用いて固定される渦巻式電極15を非水
電解液とともに電池缶内に収容してなる円筒型非水電解
液二次電池において、この粘着テープ20は支持体上に
粘着層を有してなり、この支持体はこの電解液との接触
により膨潤し、体積膨張する材料よりなるものとするこ
とにより、粘着テープの支持体が電解液との接触により
膨潤するので、非水電解液二次電池の充放電サイクル特
性を向上させることができる。Further, according to the cylindrical non-aqueous electrolyte secondary battery of the present invention, the strip negative electrode and the strip positive electrode are spirally wound so as to be laminated via the separator, and the end portion of the winding is covered with the adhesive tape 20. In a cylindrical non-aqueous electrolyte secondary battery in which the spiral electrode 15 fixed by using the non-aqueous electrolyte is housed in a battery can, the adhesive tape 20 has an adhesive layer on a support. Since the support is made of a material that swells upon contact with the electrolytic solution and expands in volume, the support of the adhesive tape swells upon contact with the electrolytic solution, so that the non-aqueous electrolyte secondary battery The charging / discharging cycle characteristic of can be improved.
【0015】また、本発明の円筒型非水電解液二次電池
によれば、帯状負極及び帯状正極をセパレータを介して
積層するように渦巻状に巻回し、その巻き終わり部を粘
着テープ20を用いて固定される渦巻式電極15を非水
電解液とともに電池缶内に収容してなる円筒型非水電解
液二次電池において、この渦巻式電極15の外径をLと
し、巻き終わり部を固定する粘着テープ20のこの外径
に沿う長さをkπLとするとき、k≧0.6であり、か
つ、この粘着テープ20は支持体上に粘着層を有してな
り、この支持体はこの電解液との接触により膨潤し、体
積膨張する材料よりなるものとすることにより、渦巻式
電極の巻き緩みを防止するために最外周に貼り付ける粘
着テープの長さを規定し、さらに、粘着テープの支持体
が電解液との接触により膨潤するので、非水電解液二次
電池の充放電サイクル特性を向上させることができる。Further, according to the cylindrical non-aqueous electrolyte secondary battery of the present invention, the strip negative electrode and the strip positive electrode are spirally wound so as to be laminated with the separator interposed therebetween, and the winding end portion is covered with the adhesive tape 20. In a cylindrical non-aqueous electrolyte secondary battery in which the spiral electrode 15 fixed by using the non-aqueous electrolyte is housed in a battery can, an outer diameter of the spiral electrode 15 is L and a winding end portion is When the length of the adhesive tape 20 to be fixed along this outer diameter is kπL, k ≧ 0.6, and the adhesive tape 20 has an adhesive layer on a support, and this support is By making it a material that swells and expands in volume upon contact with this electrolytic solution, the length of the adhesive tape to be attached to the outermost periphery is specified to prevent loosening of the spirally wound electrode. Contact of tape support with electrolyte Since more swellable, it is possible to improve the charge-discharge cycle characteristics of the nonaqueous electrolyte secondary battery.
【0016】[0016]
【実施例】以下、本発明円筒型非水電解液二次電池の一
実施例について図1〜図5を参照しながら説明しよう。EXAMPLES An example of the cylindrical non-aqueous electrolyte secondary battery of the present invention will be described below with reference to FIGS.
【0017】図1は、本例円筒型非水電解液二次電池の
渦巻式電極15の例を示し、この渦巻式電極15は、そ
れぞれ帯状である正極と負極を同じく帯状のセパレータ
の間に挟んで渦巻状に巻き込んだものである。FIG. 1 shows an example of a spiral electrode 15 of a cylindrical non-aqueous electrolyte secondary battery of the present example. The spiral electrode 15 has a strip-shaped positive electrode and a strip negative electrode between strip-shaped separators. It is sandwiched and wound in a spiral shape.
【0018】11は、負極リードを示し、この負極リー
ド11は上述の負極と電池の負極となるべき電池缶との
電気的接続をなすものである。Reference numeral 11 denotes a negative electrode lead, and this negative electrode lead 11 makes an electrical connection between the above-mentioned negative electrode and a battery can to be the negative electrode of the battery.
【0019】12は、正極リードを示し、この正極リー
ド12は上述の正極と電池の正極となるべき電池蓋との
電気的接続をなすものである。Reference numeral 12 denotes a positive electrode lead, and this positive electrode lead 12 makes an electrical connection between the above-mentioned positive electrode and a battery lid to be the positive electrode of the battery.
【0020】20は、粘着テープを示し、この粘着テー
プ20は渦巻電極15の巻き終わり部が外れないように
固定するとともに、この粘着テープ20を張力が生じる
ように貼ることにより、渦巻電極に対して圧縮力を発生
させる機能をも持つものである。Reference numeral 20 denotes an adhesive tape. The adhesive tape 20 is fixed so that the winding end portion of the spiral electrode 15 does not come off, and the adhesive tape 20 is attached so as to generate tension so that the spiral electrode 15 is attached to the spiral electrode. It also has the function of generating compressive force.
【0021】次に、本例で用いた渦巻式電極の具体的な
製造方法について説明する。本例においては、第1の本
例電池〜第4の本例電池、及び第1の比較例電池を作製
した。Next, a specific method for manufacturing the spiral electrode used in this example will be described. In this example, the first to fourth example batteries and the first comparative example battery were produced.
【0022】第1の本例電池 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、これに酸素を含む官能基を10〜20重
量%導入(いわゆる酸素架橋)した後、不活性ガス気流
中1000℃で焼成して、ガラス状炭素に近い性質を持
った炭素質材料を得た。この材料について、X線解析測
定を行った結果、(002)面の面間隔は3.8Aであ
った。またピクノメータ法により真比重を測定したとこ
ろ、1.54g/cm3 であった。この炭素材料を粉砕
し、平均粒径20μmの炭素材料粉末とした。First Example Battery Negative electrode 1 was prepared as follows. Petroleum pitch is used as a starting material, and 10 to 20% by weight of a functional group containing oxygen is introduced into this (so-called oxygen cross-linking), followed by firing at 1000 ° C. in an inert gas stream to have properties similar to glassy carbon. A carbonaceous material was obtained. As a result of X-ray analysis measurement of this material, the spacing between (002) planes was 3.8A. The true specific gravity was measured by a pycnometer method and found to be 1.54 g / cm 3 . This carbon material was crushed to obtain a carbon material powder having an average particle size of 20 μm.
【0023】このようにして得た炭素材料粉末を負極活
物質担持体とし、これを90重量部、結着材としてフッ
化ビニリデン樹脂(PVDF)10重量部を混合し、負
極合剤を調整した。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スラリー(ペースト)にし
た。The carbon material powder thus obtained was used as a negative electrode active material carrier, and 90 parts by weight of this material and 10 parts by weight of vinylidene fluoride resin (PVDF) as a binder were mixed to prepare a negative electrode mixture. . This negative electrode mixture was dispersed in N-methylpyrrolidone as a solvent to form a slurry (paste).
【0024】負極集電体として厚さ10μmの帯状の銅
箔を用い、この集電体の両面に負極合剤スラリーを塗布
し、乾燥させた後圧縮成型して帯状負極1を作製した。
成型後の合剤厚さは両面共に80μmで同一とし、電極
の幅は41.5mm、長さは720mmとした。A strip-shaped copper foil having a thickness of 10 μm was used as the negative electrode current collector, and the negative electrode mixture slurry was applied to both surfaces of this current collector, dried and then compression-molded to prepare a strip-shaped negative electrode 1.
The thickness of the mixture after molding was 80 μm on both sides, and the width of the electrode was 41.5 mm and the length was 720 mm.
【0025】正極2は次のようにして作製した。炭素リ
チウム0.5モルと炭酸コバルト1モルを混合し、90
0℃の空気中で5時間焼成してLiCoO2 を得た。得
られた材料についてX線回折測定を行った結果、JCP
DSフィルムに登録されたLiCoO2 のピークと良く
一致した。この材料を粉砕し、50%累積粒径が15μ
mのLiCoO2 粉末を得た。LiCoO2 粉末95重
量部と炭酸リチウム粉末5重量部からなる混合物を91
重量部、導電剤としてグラファイト6重量部、結着剤と
してフッ化ビニリデン樹脂3重量部を混合して正極合剤
を調整し、N−メチルピロリドンに分散させてスラリー
(ペースト状)にした。The positive electrode 2 was manufactured as follows. 90 mol of lithium carbon and 1 mol of cobalt carbonate are mixed,
LiCoO 2 was obtained by firing in air at 0 ° C. for 5 hours. X-ray diffraction measurement was performed on the obtained material, and JCP
It was in good agreement with the peak of LiCoO 2 registered in the DS film. This material is crushed to give a 50% cumulative particle size of 15μ.
m LiCoO 2 powder was obtained. A mixture of 95 parts by weight of LiCoO 2 powder and 5 parts by weight of lithium carbonate powder was added to the mixture.
By weight, 6 parts by weight of graphite as a conductive agent and 3 parts by weight of vinylidene fluoride resin as a binder were mixed to prepare a positive electrode mixture, which was dispersed in N-methylpyrrolidone to form a slurry (paste form).
【0026】正極集電体として厚さ20μmの帯状のア
ルミニウム箔を用い、この集電体の両面に均一に正極合
剤スラリーを塗布し、乾燥させた後、圧縮成型して帯状
正極2を作製した。成型後の合剤厚さは両面共に70μ
mで同一とし、電極の幅は40.5mm、長さは660
mmとした。A strip-shaped aluminum foil having a thickness of 20 μm is used as a positive electrode current collector, and the positive electrode mixture slurry is uniformly applied to both surfaces of the current collector, dried and then compression molded to produce a strip positive electrode 2. did. The thickness of the mixture after molding is 70μ on both sides.
The width of the electrode is 40.5 mm and the length is 660.
mm.
【0027】帯状負極1、帯状正極2及び厚さ25μ
m、幅44mmの微多孔性ポリプロピレンフィルムより
成るセパレータ3を負極、セパレータ、正極、セパレー
タの順に積層してから、この積層体を渦巻型に多数回巻
回した。最外周の巻き終わり部を、厚さ25μmのポリ
エステルフィルムを支持体とし、シリコン系の粘着剤を
塗布した、幅40mm、長さ41mmの粘着テープ20
で固定して外径19.6mmの電極を作製した。また、
テープは幅方向両端部を2mmずつ残して貼付け、図1
に示したような渦巻式電極を作製した。Strip negative electrode 1, strip positive electrode 2 and thickness 25 μ
A separator 3 made of a microporous polypropylene film having a width of m and a width of 44 mm was laminated in this order on the negative electrode, the separator, the positive electrode, and the separator, and then this laminated body was wound in a spiral shape many times. An adhesive tape 20 having a width of 40 mm and a length of 41 mm, which has a 25 μm-thick polyester film as a support at the outermost circumference and is coated with a silicon-based adhesive.
Then, an electrode having an outer diameter of 19.6 mm was prepared. Also,
Adhere the tape leaving 2 mm each on both ends in the width direction.
A spiral electrode as shown in 1 was produced.
【0028】このようにして作製した渦巻式電極を、図
2に示すように、ニッケルめっきを施した鉄製電池缶5
に収納した。渦巻式電極上下両面には絶縁板4を配設
し、アルミニウム製正極リード12を正極集電体から導
出して電池蓋7に、ニッケル製負極リード11を負極集
電体から導出して電池缶5に溶接した。この電池缶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中に、LiPF6 を1モル/1の割
合で溶解した電解液を注入した。As shown in FIG. 2, the spiral electrode thus prepared is plated with nickel to make an iron battery can 5.
Stored in. Insulating plates 4 are provided on both upper and lower surfaces of the spirally wound electrode, an aluminum positive electrode lead 12 is led out from the positive electrode current collector, and a nickel negative electrode lead 11 is led out from the negative electrode current collector to a battery can. Welded to 5. Into this battery can 5, an electrolyte solution in which LiPF 6 was dissolved at a ratio of 1 mol / 1 in a mixed solvent of equal volume of propylene carbonate and diethyl carbonate was injected.
【0029】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をかしめることにより、電
流遮断機構を有する安全弁装置8並びに電池蓋7を固定
し、電池内の気密性を保持させた。By caulking the battery can 5 through the insulating sealing gasket 6 whose surface is coated with asphalt, the safety valve device 8 having a current cutoff mechanism and the battery lid 7 are fixed to keep the airtightness inside the battery. .
【0030】以上のような構成で、直径20mm、高さ
50mmの円筒型非水電解液電池を試作した。A cylindrical non-aqueous electrolyte battery having a diameter of 20 mm and a height of 50 mm was manufactured as a prototype with the above structure.
【0031】第2の本例電池 渦巻式電極最外周の巻き終わり部を、幅40mm、長さ
56mmのポリエステル系テープ20を用い、幅方向両
端部を2mmずつ残して貼付けた(図3参照)こと以外
は第1の本例電池と同様の方法で、図2に示したような
直径20mm、高さ50mmの円筒型非水電解液電池を
試作した。Second Example Battery A polyester-based tape 20 having a width of 40 mm and a length of 56 mm was applied to the outermost end of the spirally wound electrode at the end of winding, leaving 2 mm at each end in the width direction (see FIG. 3). Except for the above, a cylindrical nonaqueous electrolyte battery having a diameter of 20 mm and a height of 50 mm as shown in FIG. 2 was manufactured in the same manner as the first example battery.
【0032】第3の本例電池 渦巻式電極最外周の巻き終わり部を、幅40mm、長さ
66mmのポリエステル系テープ20を用い、幅方向両
端部を2mmずつ残して、また一部が重なるように貼付
けた(図4参照)こと以外は第1の本例電池と同様の方
法で、図2に示したような直径20mm、高さ50mm
の円筒型非水電解液電池を試作した。Third Example Battery A polyester tape 20 having a width of 40 mm and a length of 66 mm is used at the outermost end of the spirally wound electrode to leave a width of 2 mm each at both ends in the width direction so that the two parts overlap each other. 20 mm in diameter and 50 mm in height as shown in FIG. 2 by the same method as the battery of the first example except that it was attached to the battery (see FIG. 4).
A cylindrical non-aqueous electrolyte battery was manufactured as a prototype.
【0033】第1の比較例電池 渦巻式電極最外周の巻き終わり部を、幅40mm、長さ
20mmのポリエステル系テープ20を用い、幅方向両
端部を2mmずつ残して貼付けた(図5参照)こと以外
は第1の本例電池と同様の方法で、図2に示したような
直径20mm、高さ50mmの円筒型非水電解液電池を
試作した。First Comparative Example Battery The outermost winding end of the spirally wound electrode was attached using a polyester tape 20 having a width of 40 mm and a length of 20 mm, leaving 2 mm at each end in the width direction (see FIG. 5). Except for the above, a cylindrical nonaqueous electrolyte battery having a diameter of 20 mm and a height of 50 mm as shown in FIG. 2 was manufactured in the same manner as the first example battery.
【0034】本例の渦巻式電極は、上述実施例による方
法ばかりでなく、他の方法によっても作製することがで
きる。The spiral electrode of this example can be manufactured not only by the method according to the above-mentioned embodiment but also by another method.
【0035】すなわち、負極としては、充放電反応に伴
いリチウム等のアルカリ金属をドープ/脱ドープ可能な
炭素材料を用いることができる。例えば、黒鉛、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、不活性ガス気流中、あるいは真空中で5
00℃以上の適当な温度で焼成したもの)、炭素繊維等
が用いられる。また、これらの材料は単独で用いる他、
複合体や混合物として用いられる。That is, as the negative electrode, it is possible to use a carbon material capable of being doped / dedoped with an alkali metal such as lithium in association with a charge / discharge reaction. For example, graphite, pyrolytic carbons, cokes (petroleum coke, pitch coke,
Coal coke, etc.), carbon black (acetylene black, etc.), glassy carbon, fired organic polymer material (organic polymer material in an inert gas stream or in a vacuum 5
Carbon fiber or the like, which is fired at a suitable temperature of 00 ° C. or higher) is used. In addition, these materials are used alone,
Used as a complex or mixture.
【0036】好ましいものとしては、(002)面の面
間隔が3.70Å以上、真密度1.70g/cm3 未満
であり、且つ空気気流中に於ける示差熱分析で700℃
以上に発熱ピークを有しない炭素質材料が用いられる。It is preferable that the (002) plane has an interplanar spacing of 3.70 Å or more and a true density of less than 1.70 g / cm 3 and a differential thermal analysis in an air stream of 700 ° C.
As described above, a carbonaceous material having no exothermic peak is used.
【0037】このような性質を有する材料としては、有
機材料を焼成等の手法により炭素化して得られる炭素質
材料が挙げられ、炭素化の出発原料としてはフルフリル
アルコールあるいはフルフラールのホモポリマー、コポ
リマーよりなるフラン樹脂が好適である。具体的には、
フラフラール+フェノール、フルフリルアルコール+ジ
メチロール尿素、フルフリルアルコール、フルフリルア
ルコール+ホルムアルデヒド、フルフリルアルコール+
フラフラール、フルフラール+ケトン類等よりなる重合
体が、非水電解液二次電池用負極剤として非常に良好な
特性を示す。Examples of the material having such a property include a carbonaceous material obtained by carbonizing an organic material by a technique such as firing, and furfuryl alcohol or furfural homopolymer or copolymer is used as a starting material for carbonization. Furan resin consisting of is preferred. In particular,
Furafural + phenol, furfuryl alcohol + dimethylol urea, furfuryl alcohol, furfuryl alcohol + formaldehyde, furfuryl alcohol +
A polymer composed of furfural, furfural, and ketones shows very good characteristics as a negative electrode agent for a non-aqueous electrolyte secondary battery.
【0038】あるいは、原料として水素/炭素原子比
0.6〜0.8の石油ピッチを用い、これに酸素を含む
官能基を導入し、いわゆる酸素架橋を施して酸素含有量
10〜20重量%の前駆体とした後、焼成して得られる
炭素質材料も好適である。Alternatively, a petroleum pitch having a hydrogen / carbon atom ratio of 0.6 to 0.8 is used as a raw material, a functional group containing oxygen is introduced into the petroleum pitch, and so-called oxygen cross-linking is performed to obtain an oxygen content of 10 to 20% by weight. A carbonaceous material obtained by firing after the precursor of is also suitable.
【0039】さらには、前記フラン樹脂や石油ピッチ等
を炭素化する際にリン化合物、あるいはホウ素化合物を
添加することにより、リチウムに対するドープ量を大き
なものとした炭素材料も使用可能である。Further, it is also possible to use a carbon material having a large doping amount with respect to lithium by adding a phosphorus compound or a boron compound when carbonizing the furan resin or petroleum pitch.
【0040】一方、正極にはLiX MO2(ただし、Mは
1種以上の遷移金属、好ましくは、CoまたはNiの少
なくとも1種をあらわし、0.05≦X≦1.10であ
る。)を含んだ活物質が使用される。かかる活物質とし
ては、LiCoO2 、LiNiO2 、LiNiy Co
(1-y) O2(但し、0.05≦X≦1.10、0<y<
1)で表される複合酸化物が挙げられる。On the other hand, Li X MO 2 (where M represents at least one transition metal, preferably at least one of Co and Ni, and 0.05 ≦ X ≦ 1.10) is used for the positive electrode. An active material containing is used. Examples of the active material include LiCoO 2 , LiNiO 2 , and LiNi y Co.
(1-y) O 2 (however, 0.05 ≦ X ≦ 1.10, 0 <y <
The complex oxide represented by 1) is mentioned.
【0041】上記複合酸化物は、たとえばリチウム、コ
バルト、ニッケル等の炭酸塩を組成に応じて混合し、酸
素存在雰囲気下600℃〜1000℃の温度範囲で焼成
することにより得られる。なお、出発原料は炭酸塩に限
定されず、水酸化物、酸化物からも同様に合成可能であ
る。The above-mentioned composite oxide is obtained, for example, by mixing carbonates such as lithium, cobalt, and nickel according to the composition and firing in a temperature range of 600 ° C. to 1000 ° C. in an atmosphere containing oxygen. The starting material is not limited to carbonate, and it can be similarly synthesized from hydroxide or oxide.
【0042】また、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、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、アセトニトリル、
プロピオリ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。電解質も従来より公知のものがいずれ
も使用でき、LiClO4 、LiAsF6、LiP
F6 、LiBF4 、LiB(C6 H5)4 、LiCl、L
iBr、CH3SO3 Li、CF3 SO3 Li等があ
る。As the electrolytic solution, 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, 1,2-dimethoxyethane, 1,2-diethoxyethane, γ-butyrolactone, tetrahydrofuran, 1,3 -Dioxolane,
4-methyl-1,3-dioxolane, diethyl ether, sulfolane, methylsulfolane, acetonitrile,
A single solvent or a mixed solvent of two or more kinds such as propiotrilyl can be used. Any known electrolyte can be used as the electrolyte, such as LiClO 4 , LiAsF 6 , and LiP.
F 6 , LiBF 4 , LiB (C 6 H 5 ) 4 , LiCl, L
There are iBr, CH 3 SO 3 Li, CF 3 SO 3 Li and the like.
【0043】渦巻式電極の最外周に貼付けるテープは種
々のものが使用可能であるが、テープ及び粘着剤の材質
が電解液の有機溶媒に対して安定であること、テープの
粘着剤の最外周に巻回されるセパレータへの粘着強度等
を考慮して選択することができる。特に、この種の電池
に一般的に用いられている電解液に対しては、ポリエチ
レン、ポリプロピレン、ポリ塩化ビニル、ポリエステ
ル、ポリイミド、フッ素樹脂系のテープの使用が望まし
い。Various tapes can be used for the outermost periphery of the spiral electrode, but the materials of the tape and the adhesive are stable to the organic solvent of the electrolytic solution, and the adhesive of the tape It can be selected in consideration of the adhesive strength to the separator wound around the outer periphery and the like. In particular, it is desirable to use polyethylene, polypropylene, polyvinyl chloride, polyester, polyimide, and fluororesin tapes for the electrolytic solution generally used in this type of battery.
【0044】次に、上述実施例において作製した電池を
各々20本用意し、上限電圧を4.2Vに設定し、1A
の定電流で2.5時間充電後、400mAの定電流で
2.75Vまで放電する充放電サイクルを繰り返した。Next, 20 batteries each prepared in the above-mentioned embodiment are prepared, the upper limit voltage is set to 4.2 V, and 1 A is set.
After charging for 2.5 hours at a constant current of 1., the charging / discharging cycle of discharging to 2.75 V at a constant current of 400 mA was repeated.
【0045】これらの電池の10サイクル目の容量(以
下、初期容量と記す)、並びに100サイクル目の容量
の平均値(各n=20)を、各電極の巻き終わり部の固
定に用いた粘着テープ長さと共に、表1に示した。The capacity at the 10th cycle of these batteries (hereinafter referred to as the initial capacity) and the average value of the capacity at the 100th cycle (each n = 20) were used to fix the winding end portion of each electrode. It is shown in Table 1 together with the tape length.
【0046】[0046]
【表1】 [Table 1]
【0047】表1に示すように、第1〜第3の本例電池
は従来の方法による第1の比較例電池に比べ、サイクル
経過後の容量が大きく、充放電サイクル進行に伴う劣化
率が小さい。As shown in Table 1, the first to third batteries of the present example have larger capacities after the passage of the cycle and the deterioration rate with the progress of the charge / discharge cycle as compared with the first comparative battery of the conventional method. small.
【0048】以上示したように、本例電池は高容量が得
られ、サイクル寿命に優れる。なお、実施例の説明には
一枚の粘着テープで固定した場合を示したが、合計の長
さが本発明の範囲にはいるように、複数枚に分割して断
続的に貼ることも可能である。この場合、複数枚のうち
の一枚が巻き終わり部の固定に使われる。As shown above, the battery of this example has a high capacity and an excellent cycle life. In the description of the examples, the case of fixing with one piece of adhesive tape was shown, but it is also possible to divide it into a plurality of pieces and attach them intermittently so that the total length falls within the scope of the present invention. Is. In this case, one of the plurality of sheets is used to fix the winding end portion.
【0049】また、説明には粘着テープの幅は、電極
(セパレータ)のほぼ全域を覆うものを用いたが、必ず
しもこの幅が確保できなくともよい。但し、電極幅に対
して40%以上の部分を覆うことが望ましい。この場
合、テープの貼付け方法としては、1枚のテープでも複
数のテープを使用しても良く、複数のテープにより固定
する場合には、各テープの幅の合計が電極幅に対して4
0%以上であれば良い。In the description, the width of the adhesive tape covers almost the entire area of the electrode (separator), but it is not always necessary to secure this width. However, it is desirable to cover a portion of 40% or more of the electrode width. In this case, as a method of attaching the tapes, one tape or a plurality of tapes may be used. When the tapes are fixed by a plurality of tapes, the total width of each tape is 4 with respect to the electrode width.
It should be 0% or more.
【0050】以上のことから、本例によれば、渦巻式電
極の巻き緩みを防止するために最外周に貼り付ける粘着
テープの長さを規定することにより、円筒型非水電解液
二次電池の充放電サイクル特性を向上させることができ
る。From the above, according to this example, the length of the adhesive tape attached to the outermost periphery in order to prevent the loosening of the spirally wound electrode is regulated, whereby the cylindrical non-aqueous electrolyte secondary battery is provided. The charging / discharging cycle characteristic of can be improved.
【0051】なお、上述実施例においては、渦巻式電極
の外径をLとし、巻き終わり部を固定する粘着テープの
外径に沿う長さをkπLとするとき、k≧0.6のもの
について検討を行った。In the above embodiment, when the outer diameter of the spiral electrode is L and the length along the outer diameter of the adhesive tape for fixing the winding end portion is kπL, k ≧ 0.6. Study was carried out.
【0052】実施例の厚さ25μmの支持体を用いた場
合、k≧2にしても効果は変わらず、また、kを余り大
きくするとその体積分だけ電極の体積を減らすことにな
る。しかし、粘着テープをさらに薄いものを用いれば、
kを2以上にすることも可能である。When the support having a thickness of 25 μm of the embodiment is used, the effect does not change even if k ≧ 2, and if k is made too large, the volume of the electrode is reduced by the volume. However, if you use a thinner adhesive tape,
It is also possible that k is 2 or more.
【0053】次に、本例円筒型非水電解液二次電池の他
の実施例について図6〜図10を参照しながら説明しよ
う。Next, another embodiment of the cylindrical non-aqueous electrolyte secondary battery of this embodiment will be described with reference to FIGS. 6 to 10.
【0054】図6は、本例円筒型非水電解液二次電池の
他の実施例に用いた渦巻式電極を示すものである。この
渦巻式電極の構成は上述の実施例とほぼ同じものである
が、上述の実施例においては、粘着テープとして電解液
により膨潤しないものを用いていたが、本例では膨潤性
を有する粘着テープを用いたものである。FIG. 6 shows a spiral electrode used in another example of the cylindrical nonaqueous electrolyte secondary battery of this example. Although the structure of this spiral electrode is almost the same as that of the above-mentioned embodiment, in the above-mentioned embodiment, the adhesive tape which does not swell by the electrolytic solution was used, but in this embodiment, the adhesive tape having swelling property. Is used.
【0055】次に、本例で用いた渦巻式電極の具体的な
製造方法について説明する。本例においては、第4の本
例電池〜第6の本例電池、及び第2の比較例電池を作製
した。Next, a specific method for manufacturing the spiral electrode used in this example will be described. In this example, the fourth to sixth example batteries and the second comparative example battery were produced.
【0056】ここで、負極1、負極集電体9、正極2、
及び正極集電体10は、上述した実施例での方法と同じ
方法により作製した。Here, the negative electrode 1, the negative electrode current collector 9, the positive electrode 2,
The positive electrode current collector 10 and the positive electrode current collector 10 were manufactured by the same method as that of the above-described example.
【0057】第4の本例電池 帯状負極1、帯状正極2及び厚さ25μm、幅44mm
の微多孔性ポリプロピレンフィルムより成るセパレータ
3を負極、セパレータ、正極、セパレータの順に積層し
てから、この積層体を渦巻型に多数回巻回した。最外周
の巻き終わり部を、厚さ30μmのフッ化ビニリデン樹
脂フィルムを支持体とし、アクリル樹脂系の粘着剤を塗
布した、幅40mm、長さ56mmの粘着テープ20で
固定して外径19.6mmの電極を作製した。また、テ
ープは幅方向両端部を2mmずつ残して貼付け、図6に
示したような渦巻式電極を作製した。Fourth Example Battery Band-shaped negative electrode 1, band-shaped positive electrode 2 and thickness 25 μm, width 44 mm
The negative electrode, the separator, the positive electrode, and the separator were laminated in this order on the separator 3 made of the microporous polypropylene film, and then the laminated body was wound in a spiral shape many times. The end of the outermost winding is fixed with an adhesive tape 20 having a width of 40 mm and a length of 56 mm, which is coated with an acrylic resin-based pressure sensitive adhesive, using a vinylidene fluoride resin film having a thickness of 30 μm as a support, and has an outer diameter of 19. A 6 mm electrode was prepared. Further, the tape was attached while leaving both widthwise end portions of 2 mm each, to produce a spiral electrode as shown in FIG.
【0058】なお、このベース・フィルムの膨潤性をみ
るために、50mm×60mmの試験片とし、これを使
用電解液に6時間浸せきしこのベース・フィルムの体積
膨張率を測定した結果、これは約40%であった。In order to check the swelling property of this base film, a test piece of 50 mm × 60 mm was used, which was dipped in the electrolyte used for 6 hours and the volume expansion coefficient of this base film was measured. It was about 40%.
【0059】このようにして作製した渦巻式電極を、図
7に示すように、ニッケルめっきを施した鉄製電池缶5
に収納した。渦巻式電極上下両面には絶縁板4を配設
し、アルミニウム製正極リード12を正極集電体から導
出して電池蓋7に、ニッケル製負極リード11を負極集
電体から導出して電池缶5に溶接した。この電池缶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中に、LiPF6 を1モル/1の割
合で溶解した電解液を注入した。As shown in FIG. 7, the spiral electrode thus produced was plated with nickel to make an iron battery can 5.
Stored in. Insulating plates 4 are provided on both upper and lower surfaces of the spirally wound electrode, an aluminum positive electrode lead 12 is led out from the positive electrode current collector, and a nickel negative electrode lead 11 is led out from the negative electrode current collector to a battery can. Welded to 5. Into this battery can 5, an electrolyte solution in which LiPF 6 was dissolved at a ratio of 1 mol / 1 in a mixed solvent of equal volume of propylene carbonate and diethyl carbonate was injected.
【0060】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をかしめることにより、電
流遮断機構を有する安全弁装置8並びに電池蓋7を固定
し、電池内の気密性を保持させた。By caulking the battery can 5 through the insulating sealing gasket 6 whose surface was coated with asphalt, the safety valve device 8 having the current cutoff mechanism and the battery lid 7 were fixed to maintain the airtightness inside the battery. .
【0061】以上のような構成で、直径20mm、高さ
50mmの円筒型非水電解液電池を試作した。A cylindrical non-aqueous electrolyte battery having a diameter of 20 mm and a height of 50 mm was manufactured as a prototype with the above-mentioned structure.
【0062】第5の本例電池 電極最外周の巻き終わり部を固定する粘着テープにおけ
るベース・フィルムの材質を、架橋ポリエチレン・オキ
サイド樹脂としたこと以外は第4の本例電池と同じ方法
で、図6に示したような渦巻式電極を作製し、図7に示
したような直径20mm、高さ50mmの円筒型非水電
解液電池を試作した。なお、ベース・フィルムの膨潤に
よる体積膨張率は約820%であった。Fifth Present Example Battery The same method as in the fourth present example battery except that the material of the base film in the adhesive tape for fixing the winding end portion of the outermost periphery of the electrode is a crosslinked polyethylene oxide resin. A spiral electrode as shown in FIG. 6 was produced, and a cylindrical nonaqueous electrolyte battery having a diameter of 20 mm and a height of 50 mm as shown in FIG. The volume expansion coefficient due to the swelling of the base film was about 820%.
【0063】第6の本例電池 電極最外周の巻き終わり部を固定する粘着テープにおけ
るベース・フィルムの材質を、一軸延伸した塩化ビニル
樹脂としたこと以外は第4の本例電池と同じ方法で、図
6に示したような渦巻式電極を作製し、図7に示したよ
うな直径20mm、高さ50mmの円筒型非水電解液電
池を試作した。なお、ベース・フィルムの膨潤による体
積膨張率は約20%であった。Sixth Example Battery The same method as in the fourth example battery except that the material of the base film of the adhesive tape for fixing the winding end portion of the outermost periphery of the electrode is uniaxially stretched vinyl chloride resin. A spiral type electrode as shown in FIG. 6 was produced, and a cylindrical non-aqueous electrolyte battery having a diameter of 20 mm and a height of 50 mm as shown in FIG. The volume expansion coefficient due to the swelling of the base film was about 20%.
【0064】第2の比較例電池 電極最外周の巻き終わり部を固定する粘着テープにおけ
るベース・フィルムの材質を、ポリエステル樹脂とした
こと以外は第4の本例電池と同じ方法で、図8に示した
ような渦巻式電極を作製し、図7に示したような直径2
0mm、高さ50mmの円筒型非水電解液電池を試作し
た。Second Comparative Example Battery The same method as in the fourth example battery except that the material of the base film in the adhesive tape for fixing the winding end portion of the outermost periphery of the electrode was polyester resin was used. A spiral type electrode as shown in FIG.
A cylindrical non-aqueous electrolyte battery having a height of 0 mm and a height of 50 mm was manufactured as a prototype.
【0065】本例の渦巻式電極に用いた粘着テープは、
上述実施例による方法ばかりでなく、他の方法によって
も作製することができる。The adhesive tape used for the spiral electrode of this example is
It can be manufactured not only by the method according to the above-described embodiment but also by other methods.
【0066】すなわち、渦巻式電極の最外周の巻き終わ
り部を固定するための粘着テープとしては、電解液との
接触により、ベース・フィルムが膨潤し体積膨張する材
料を種々使用することができる。That is, as the adhesive tape for fixing the outermost winding end portion of the spirally wound electrode, various materials can be used in which the base film swells and expands in volume upon contact with the electrolytic solution.
【0067】ベース・フィルムの膨潤は、材料の溶解等
によって起きる変化、材質の化学的な反応によって起き
る変化、延伸等の機械的前処理を行った材料の復元力に
よって起きる変化等による結果として現れる現象であ
る。The swelling of the base film appears as a result of a change caused by dissolution of the material, a change caused by a chemical reaction of the material, a change caused by the restoring force of the material subjected to mechanical pretreatment such as stretching, and the like. It is a phenomenon.
【0068】ベース・フィルムとなる高分子化合物の、
溶解による膨潤し易さを支配する因子としては、電解液
の有機溶媒に対する誘電率や極性等が挙げられる。ま
た、化学的変化による膨潤とは、電解液中の溶媒、溶質
がベース・フィルムとなる高分子化合物と化学反応し、
新らたな物質が生成することにより、体積が膨張するも
の等をいう。さらに、機械的な性質による膨潤とは、延
伸等の機械的前処理を行ったベース・フィルムが、長さ
方向に収縮することにより、処理前の厚さに復元する結
果生じるもの等をいう。いずれの場合も最適なベース・
フィルムの材質は、使用する電解液の種類によって決定
される。Of the high molecular compound to be the base film,
Factors that control the ease of swelling due to dissolution include the dielectric constant and polarity of the electrolytic solution with respect to the organic solvent. In addition, swelling due to chemical changes means that the solvent and solute in the electrolytic solution chemically react with the polymer compound that becomes the base film,
It refers to a material whose volume expands due to the production of a new material. Further, the swelling due to mechanical properties means that the base film that has been subjected to mechanical pretreatment such as stretching contracts in the lengthwise direction to restore the thickness before the treatment. The best base for either case
The material of the film is determined by the type of electrolyte used.
【0069】ここで、膨潤というのは、直接フィルムの
厚さが増加するものだけでなく、フィルム本来の厚さに
はほとんど変化は見られないが、長さ方向への増加がシ
ワとなって現れ、実質的に厚さが増加した場合と同様の
効果が得られるものも含まれる。Here, the swelling means not only the increase in the thickness of the film directly, but almost no change in the original thickness of the film is observed, but the increase in the length direction causes wrinkles. Those that appear and have the same effect as when the thickness is increased are also included.
【0070】また、テープに塗布される粘着剤は最外周
に巻回されるセパレータへの粘着強度等を考慮して種々
選択することができるが、用いる電解液の有機溶媒に対
して安定であることが望ましい。The pressure-sensitive adhesive applied to the tape can be variously selected in consideration of the pressure-sensitive adhesive strength to the separator wound on the outermost periphery, but is stable to the organic solvent of the electrolytic solution used. Is desirable.
【0071】次に、上述実施例において作製した電池と
各々20本用意し、上限電圧を4.2Vに設定し、1A
の定電流で2.5時間充電後、400mAの定電流で
2.75Vまで放電する充放電サイクルを繰り返した。
なお、電極を間に挿入する時点においては、電極外径〜
缶内径間に生産上十分なクリアランスが確保されている
ため、第4〜第6の本例電池、第2の比較例電池共に挿
入不良は発生しなかった。Next, 20 batteries each prepared in the above-mentioned embodiment and 20 batteries were prepared, the upper limit voltage was set to 4.2 V, and 1 A was set.
After charging for 2.5 hours at a constant current of 1., the charging / discharging cycle of discharging up to 2.75 V at a constant current of 400 mA was repeated.
In addition, at the time of inserting the electrode between the electrode outer diameter ~
Since a sufficient clearance was secured between the inner diameters of the cans for production, no defective insertion occurred in both the fourth to sixth batteries of this example and the second comparative battery.
【0072】これらの電池の10サイクル目の容量(初
期容量)、並びに100サイクル目の容量の平均値(n
=20)を、表2に示した。また、100サイクル経過
後の電池を分解し、各電極の巻き終わり部の固定に用い
た粘着テープのベース・フィルムの膨潤の有無を調べ、
表2に併せて示した。The capacity of the 10th cycle (initial capacity) of these batteries and the average value of the capacity of the 100th cycle (n
= 20) is shown in Table 2. Also, after 100 cycles, the battery was disassembled, and the presence or absence of swelling of the base film of the adhesive tape used for fixing the winding end portion of each electrode was examined.
It is also shown in Table 2.
【0073】[0073]
【表2】 [Table 2]
【0074】表2に示すように、本発明電池は従来の方
法による比較例電池に比べ、サイクル経過後の容量が大
きく、充放電サイクル進行に伴う劣化率が小さい。これ
は、100サイクル経過後の第4の本例電池より取り出
した粘着テープのベース・フィルムの外観(図9参照)
からもわかるように、電解液との接触により膨潤したフ
ィルムが電極外径と電池缶内径とのクリアランスを埋
め、さらに電極に対し外周方向から中心に向けて加圧す
る力が働き、円滑に電極反応が行われたためと考えられ
る。なお、第2の比較例電池から取り出したベースフィ
ルムの外観を図10に示した。As shown in Table 2, the battery of the present invention has a large capacity after a lapse of cycles and a small deterioration rate due to the progress of charge / discharge cycles, as compared with the battery of the comparative example by the conventional method. This is the appearance of the base film of the adhesive tape taken out from the battery of Example 4 after 100 cycles (see FIG. 9).
As can be seen from the figure, the film swollen by the contact with the electrolyte fills the clearance between the outer diameter of the electrode and the inner diameter of the battery can, and the force that presses the electrode from the outer peripheral direction toward the center works smoothly, and the electrode reaction smoothly. It is thought that this was done. The appearance of the base film taken out from the second comparative battery is shown in FIG.
【0075】本例によれば高容量で、サイクル特性に優
れた電池が生産性よく量産できる。なお、実施例の説明
には電解液に対し膨潤する材質のベース・フィルムから
なる一枚の粘着テープで固定した場合を示したが、複数
の材質からなる粘着テープを併用したり、非膨潤性テー
プで固定した後、その外周に更に膨潤性テープを貼付け
たり、あるいは膨潤性フィルムを電極〜缶間に挿入し同
様の効果を期待することもできる。According to this example, a battery having a high capacity and excellent cycle characteristics can be mass-produced with high productivity. In the description of the examples, the case of fixing with one piece of adhesive tape made of a base film made of a material that swells in an electrolytic solution is shown. After fixing with a tape, a swelling tape may be further attached to the outer periphery thereof, or a swelling film may be inserted between the electrode and the can to expect the same effect.
【0076】なお、上述の実施例で用いたベース・フィ
ルムの膨潤性については、常温で1昼夜このベース・フ
ィルムを使用電解液に浸せきした結果、体積膨張率が5
%以上であることが好ましく、また10%以上であれば
さらに好ましい効果が得られる。Regarding the swelling property of the base film used in the above-mentioned examples, the volume expansion coefficient was 5 as a result of immersing the base film in an electrolyte solution at room temperature for one day.
% Or more, and if 10% or more, further preferable effects can be obtained.
【0077】以上のことから、本例によれば、渦巻式電
極の巻き緩みを防止するために最外周に貼り付ける粘着
テープのベース・フィルムの材質を、電解液との接触に
より膨潤する材料とすることにより、非水電解液二次電
池の充放電サイクル特性を向上させることができる。ま
た、粘着テープの長さを種々の長さにして用いることも
勿論できる。From the above, according to this example, the material of the base film of the adhesive tape attached to the outermost periphery in order to prevent the spirally wound electrode from being loosened is changed to the material which swells by contact with the electrolytic solution. By doing so, the charge / discharge cycle characteristics of the non-aqueous electrolyte secondary battery can be improved. Further, it is of course possible to use the adhesive tape with various lengths.
【0078】なお、本発明は上述の実施例に限らず本発
明の要旨を逸脱することなくその他種々の構成を採り得
ることはもちろんである。The present invention is not limited to the above-mentioned embodiments, and it goes without saying that various other configurations can be adopted without departing from the gist of the present invention.
【0079】[0079]
【発明の効果】以上説明したように、本発明によれば、
渦巻式電極の最外周に貼り付ける粘着テープの長さを規
定することにより、また、粘着テープのベース・フィル
ムの材質を電解液との接触により膨潤する材料とするこ
とにより、円筒型非水電解液二次電池の充放電サイクル
特性を向上させることができる。As described above, according to the present invention,
By defining the length of the adhesive tape that is attached to the outermost circumference of the spiral electrode and by making the material of the base film of the adhesive tape a material that swells when contacted with the electrolytic solution, The charge / discharge cycle characteristics of the liquid secondary battery can be improved.
【図1】本発明円筒型非水電解液二次電池の一実施例の
渦巻式電極を示す構成図である。FIG. 1 is a configuration diagram showing a spiral electrode of an example of a cylindrical non-aqueous electrolyte secondary battery of the present invention.
【図2】本発明円筒型非水電解液二次電池の一実施例を
示す断面図である。FIG. 2 is a cross-sectional view showing an example of the cylindrical non-aqueous electrolyte secondary battery of the present invention.
【図3】本発明円筒型非水電解液二次電池の一実施例の
渦巻式電極を示す斜視図である。FIG. 3 is a perspective view showing a spiral electrode of an example of the cylindrical non-aqueous electrolyte secondary battery of the present invention.
【図4】本発明円筒型非水電解液二次電池の一実施例の
渦巻式電極を示す構成図である。FIG. 4 is a configuration diagram showing a spiral electrode of an example of the cylindrical non-aqueous electrolyte secondary battery of the present invention.
【図5】円筒型非水電解液二次電池の比較例の渦巻式電
極を示す斜視図である。FIG. 5 is a perspective view showing a spiral electrode of a comparative example of a cylindrical non-aqueous electrolyte secondary battery.
【図6】本発明円筒型非水電解液二次電池の他の実施例
の渦巻式電極を示す構成図である。FIG. 6 is a configuration diagram showing a spiral electrode of another embodiment of the cylindrical non-aqueous electrolyte secondary battery of the present invention.
【図7】本発明円筒型非水電解液二次電池の他の実施例
を示す断面図である。FIG. 7 is a sectional view showing another embodiment of the cylindrical non-aqueous electrolyte secondary battery of the present invention.
【図8】円筒型非水電解液二次電池の比較例の渦巻式電
極を示す斜視図である。FIG. 8 is a perspective view showing a spiral electrode of a comparative example of a cylindrical non-aqueous electrolyte secondary battery.
【図9】本例の渦巻式電極から取り出した粘着テープの
ベース・フィルムを示す説明図である。FIG. 9 is an explanatory diagram showing a base film of an adhesive tape taken out from the spiral electrode of this example.
【図10】比較例の渦巻式電極から取り出した粘着テー
プのベース・フィルムを示す説明図である。FIG. 10 is an explanatory diagram showing a base film of an adhesive tape taken out from a spiral electrode of a comparative example.
11 負極リード 12 正極リード 15 渦巻式電極 20 粘着テープ 11 Negative electrode lead 12 Positive electrode lead 15 Swirl type electrode 20 Adhesive tape
フロントページの続き (72)発明者 小丸 篤雄 福島県郡山市日和田町高倉字下杉下1−1 株式会社ソニー・エナジー・テック郡山 工場内 (72)発明者 伊達 尚幸 福島県郡山市日和田町高倉字下杉下1−1 株式会社ソニー・エナジー・テック郡山 工場内Continued Front Page (72) Inventor Atsushi Komaru 1-1 Takashimo Shimosugishita, Takakura, Hiwada-cho, Koriyama-shi, Fukushima Prefecture Sony Energy Tech Co., Ltd. Koriyama Plant (72) Naoyuki Date Date Takakura, Hiwada-cho, Koriyama-shi, Fukushima Prefecture 1-1 Shimoshita Sugishita Sony Energy Tech Koriyama Factory
Claims (3)
して積層するように渦巻状に巻回し、その巻き終わり部
を粘着テープを用いて固定される渦巻式電極を非水電解
液とともに電池缶内に収容してなる円筒型非水電解液二
次電池において、 上記渦巻式電極の外径をLとし、巻き終わり部を固定す
る粘着テープの該外径に沿う長さをkπLとするとき、
k≧0.6であることを特徴とする円筒型非水電解液二
次電池。1. A spirally wound electrode in which a strip negative electrode and a strip positive electrode are spirally wound so as to be laminated with a separator interposed therebetween, and a winding end portion is fixed with an adhesive tape in a battery can together with a non-aqueous electrolyte. In the cylindrical non-aqueous electrolyte secondary battery housed in, when the outer diameter of the spiral electrode is L and the length along the outer diameter of the adhesive tape for fixing the winding end portion is kπL,
A cylindrical non-aqueous electrolyte secondary battery, wherein k ≧ 0.6.
して積層するように渦巻状に巻回し、その巻き終わり部
を粘着テープを用いて固定される渦巻式電極を非水電解
液とともに電池缶内に収容してなる円筒型非水電解液二
次電池において、 上記粘着テープは支持体上に粘着層を有してなり、該支
持体は上記電解液との接触により膨潤し、体積膨張する
材料よりなることを特徴とする円筒型非水電解液二次電
池。2. A spirally wound electrode in which a strip negative electrode and a strip positive electrode are spirally wound so as to be laminated with a separator interposed therebetween, and a winding end portion is fixed with an adhesive tape in a battery can together with a non-aqueous electrolyte. In the cylindrical non-aqueous electrolyte secondary battery housed in, the pressure-sensitive adhesive tape has a pressure-sensitive adhesive layer on a support, and the support swells by contact with the electrolyte and expands in volume. A cylindrical non-aqueous electrolyte secondary battery comprising:
して積層するように渦巻状に巻回し、その巻き終わり部
を粘着テープを用いて固定される渦巻式電極を非水電解
液とともに電池缶内に収容してなる円筒型非水電解液二
次電池において、 上記渦巻式電極の外径をLとし、巻き終わり部を固定す
る粘着テープの該外径に沿う長さをkπLとするとき、
k≧0.6であり、 かつ、上記粘着テープは支持体上に粘着層を有してな
り、該支持体は上記電解液との接触により膨潤し、体積
膨張する材料よりなることを特徴とする円筒型非水電解
液二次電池。3. A spiral wound electrode in which a strip negative electrode and a strip positive electrode are spirally wound so as to be laminated via a separator, and the end of the winding is fixed with an adhesive tape in a battery can together with a non-aqueous electrolyte. In the cylindrical non-aqueous electrolyte secondary battery housed in, when the outer diameter of the spiral electrode is L and the length along the outer diameter of the adhesive tape for fixing the winding end portion is kπL,
k ≧ 0.6, and the pressure-sensitive adhesive tape has a pressure-sensitive adhesive layer on a support, and the support is made of a material that swells upon contact with the electrolyte and expands in volume. Cylindrical non-aqueous electrolyte secondary battery.
Priority Applications (1)
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JP29288092A JP3321853B2 (en) | 1992-10-30 | 1992-10-30 | Non-aqueous electrolyte secondary battery |
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Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
JP29288092A JP3321853B2 (en) | 1992-10-30 | 1992-10-30 | Non-aqueous electrolyte secondary battery |
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JP3321853B2 JP3321853B2 (en) | 2002-09-09 |
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Cited By (26)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
EP1104040A1 (en) * | 1999-11-25 | 2001-05-30 | NEC Mobile Energy Corporation | Nonaqueous electrolyte secondary battery |
JP2003178792A (en) * | 2001-11-06 | 2003-06-27 | Samsung Sdi Co Ltd | Secondary battery |
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-
1992
- 1992-10-30 JP JP29288092A patent/JP3321853B2/en not_active Expired - Lifetime
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