JPH08321312A - Nonaqueous electrolyte battery - Google Patents
Nonaqueous electrolyte batteryInfo
- Publication number
- JPH08321312A JPH08321312A JP7150844A JP15084495A JPH08321312A JP H08321312 A JPH08321312 A JP H08321312A JP 7150844 A JP7150844 A JP 7150844A JP 15084495 A JP15084495 A JP 15084495A JP H08321312 A JPH08321312 A JP H08321312A
- Authority
- JP
- Japan
- Prior art keywords
- aqueous electrolyte
- dimethyl
- lithium
- negative electrode
- 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.)
- Pending
Links
Classifications
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Landscapes
- Primary Cells (AREA)
- Secondary Cells (AREA)
Abstract
Description
【０００１】[0001]
【産業上の利用分野】本発明は、非水電解液電池に係わ
り、詳しくは非水電解液電池の保存特性を改善すること
を目的とした、非水電解液の改良に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a non-aqueous electrolyte battery, and more particularly to an improvement in a non-aqueous electrolyte solution for the purpose of improving the storage characteristics of the non-aqueous electrolyte battery.
【０００２】[0002]
【従来の技術及び発明が解決しようとする課題】近年、
リチウムを活物質とする負極を備える非水電解液電池
が、正極の活物質を適宜選定することにより高容量化が
可能なことから注目されている。2. Description of the Related Art In recent years,
A non-aqueous electrolyte battery including a negative electrode using lithium as an active material is drawing attention because it can have a high capacity by appropriately selecting the positive electrode active material.
【０００３】ところで、リチウムを活物質とする負極と
しては、金属リチウム、リチウム合金、炭素材料などが
提案されている。By the way, as a negative electrode using lithium as an active material, metallic lithium, lithium alloys, carbon materials, etc. have been proposed.
【０００４】しかしながら、これらの負極材料は一般に
保存中に非水電解液と反応し易く、このためリチウムを
負極の活物質とする非水電解液電池には、長期間保存す
ると自己放電により放電容量が著しく減少するという問
題がある。However, these negative electrode materials generally easily react with the non-aqueous electrolyte solution during storage, and therefore a non-aqueous electrolyte battery using lithium as an active material of the negative electrode will have a discharge capacity due to self-discharge when stored for a long period of time. Is significantly reduced.
【０００５】本発明は、この問題を解決するべくなされ
たものであって、その目的とするところは、負極と非水
電解液との反応に起因する自己放電を抑制することによ
り、優れた保存特性を有する非水電解液電池を提供する
にある。The present invention has been made to solve this problem, and an object thereof is to suppress self-discharge caused by a reaction between a negative electrode and a non-aqueous electrolyte, thereby achieving excellent preservation. A non-aqueous electrolyte battery having characteristics is provided.
【０００６】[0006]
【課題を解決するための手段】上記目的を達成するため
の本発明に係る非水電解液電池（本発明電池）は、正極
と、リチウムを活物質とする負極と、エチレンカーボネ
ート、プロピレンカーボネート及びブチレンカーボネー
トよりなる群から選ばれた少なくとも一種の高誘電率溶
媒にトリフルオロメタンスルホン酸リチウム又はヘキサ
フルオロリン酸リチウムを溶かしてなる非水電解液と、
セパレータとを備える非水電解液電池であって、前記非
水電解液が、トリエチルアミン、ｎ−ブチルアミン、ア
ニリン、トリメチルヒドロキシルアミン、１−ジメチル
アミノ−２−メトキシエタン、アセトニトリル、アクリ
ロニトリル、３−メトキシプロピオニトリル、ベンゾニ
トリル、ニトロメタン、ニトロエタン、Ｎ，Ｎ−ジメチ
ルアセトアミド、Ｎ，Ｎ−ジメチルホルムアミド、ホル
ムアミド、Ｎ−メチル−２−ピロリドン、Ｎ，Ｎ'−ジ
メチルイミダゾリジノン、イソキサゾール、３，５−ジ
メチルイソキサゾール、３−メチル−２−オキサゾリド
ン、１，２，３−オキサジアゾール、Ｎ−メチルモルホ
リン、ジメチルスルフィド、エチルメチルスルフィド、
２−メチルチオフェン、１−ブタンチオール、ベンゼン
チオール、ジメチルサルフェート、ジエチルサルフェー
ト、ジメチルサルファイト、ジエチルサルファイト、ブ
タジエンスルホン、３−メチルスルホレン、１，４−チ
オキサン、フェノキサチイン、１，４−チアジン、チオ
モルホリン、ピリジン、１，３−ジメチル−２−イミダ
ゾリジノン、ジメチルスルホキシド、ジメチルスルホ
ン、メチルエチルスルホネート及びジメチルスルフィナ
イトよりなる群から選ばれた少なくとも１種の添加剤を
１〜２０体積％含有する。A non-aqueous electrolyte battery according to the present invention (a battery according to the present invention) for achieving the above object comprises a positive electrode, a negative electrode using lithium as an active material, ethylene carbonate, propylene carbonate and A nonaqueous electrolytic solution obtained by dissolving lithium trifluoromethanesulfonate or lithium hexafluorophosphate in at least one high dielectric constant solvent selected from the group consisting of butylene carbonate,
A non-aqueous electrolyte battery comprising a separator, wherein the non-aqueous electrolyte is triethylamine, n-butylamine, aniline, trimethylhydroxylamine, 1-dimethylamino-2-methoxyethane, acetonitrile, acrylonitrile, 3-methoxyproton. Pionitoriru, benzonitrile, nitromethane, nitroethane, N, N- dimethylacetamide, N, N- dimethylformamide, formamide, N- methyl-2-pyrrolidone, N, N '- dimethyl imidazolidinone, isoxazole, 3,5 Dimethylisoxazole, 3-methyl-2-oxazolidone, 1,2,3-oxadiazole, N-methylmorpholine, dimethyl sulfide, ethyl methyl sulfide,
2-methylthiophene, 1-butanethiol, benzenethiol, dimethylsulfate, diethylsulfate, dimethylsulfite, diethylsulfite, butadienesulfone, 3-methylsulfolene, 1,4-thioxane, phenoxathiin, 1,4- 1 to 20 of at least one additive selected from the group consisting of thiazine, thiomorpholine, pyridine, 1,3-dimethyl-2-imidazolidinone, dimethyl sulfoxide, dimethyl sulfone, methyl ethyl sulfonate and dimethyl sulfinite. Contains by volume%.
【０００７】本発明電池の非水電解液は特定の添加剤を
１〜２０体積％含有する。添加剤含有率がこの範囲を外
れると、保存特性が向上しにくくなる。The non-aqueous electrolyte of the battery of the present invention contains 1 to 20 volume% of a specific additive. If the additive content is out of this range, it becomes difficult to improve the storage characteristics.
【０００８】非水電解液の溶媒として、上記高誘電率溶
媒に１，２−ジメトキシエタンを加えた混合溶媒を使用
すれば、保存特性をさらに改善することができる。その
場合の高誘電率溶媒と１，２−ジメトキシエタンとの好
適な含有比は、体積比で３：７〜７：３の範囲である。If a mixed solvent obtained by adding 1,2-dimethoxyethane to the above high dielectric constant solvent is used as the solvent for the non-aqueous electrolyte, the storage characteristics can be further improved. In that case, the preferable content ratio of the high dielectric constant solvent and 1,2-dimethoxyethane is in the range of 3: 7 to 7: 3 by volume ratio.
【０００９】リチウムを活物質とする負極の具体例とし
ては、リチウム合金（リチウム・アルミニウム合金、リ
チウム・鉛合金、リチウム・錫合金など）、金属酸化物
（ＬｉＮｂ2 Ｏ5 など）又は炭素材料（黒鉛、コーク
ス、有機物焼成体など）を負極材料に使用したものが挙
げられる。Specific examples of the negative electrode using lithium as an active material include lithium alloys (lithium-aluminum alloys, lithium-lead alloys, lithium-tin alloys, etc.), metal oxides (LiNb 2 O 5, etc.), or carbon materials ( Examples of the negative electrode material include graphite, coke, and a fired organic material.
【００１０】本発明は、特定の負極と特定の非水電解液
とを備える非水電解液電池の保存特性を改善するべく、
非水電解液として特定の添加剤を所定量含有するものを
使用した点にその特徴が有る。したがって、正極、セパ
レータなどの電池を構成する他の部材については、非水
電解液電池用として従来提案乃至実用されている種々の
ものを使用することができる。また、本発明は、一次電
池及び二次電池の両方に適用可能なものである。The present invention aims to improve the storage characteristics of a non-aqueous electrolyte battery comprising a specific negative electrode and a specific non-aqueous electrolyte.
The characteristic is that a non-aqueous electrolyte containing a specific additive in a predetermined amount was used. Therefore, as the other members constituting the battery such as the positive electrode and the separator, various members which have been proposed or put into practical use for the non-aqueous electrolyte battery can be used. Further, the present invention is applicable to both primary batteries and secondary batteries.
【００１１】[0011]
【作用】非水電解液に含有させた特定の添加剤と、非水
電解液中の溶媒・溶質及び負極中のリチウムとが反応し
て、負極表面に被膜が形成される。この被膜により、負
極と非水電解液との反応が起こりにくくなるので、自己
放電が抑制される。その結果、長期間保存した場合でも
放電容量が減少しにくくなる（保存特性の向上）。な
お、被膜は電子電導性が良好であるので、負極に被膜が
形成されることにより負極における電極反応が阻害され
ることはない。The specific additive contained in the non-aqueous electrolytic solution reacts with the solvent / solute in the non-aqueous electrolytic solution and lithium in the negative electrode to form a film on the surface of the negative electrode. This coating makes it difficult for the reaction between the negative electrode and the non-aqueous electrolyte to occur, so that self-discharge is suppressed. As a result, the discharge capacity is less likely to decrease even after long-term storage (improvement of storage characteristics). Since the coating has good electron conductivity, the coating reaction on the negative electrode does not hinder the electrode reaction at the negative electrode.
【００１２】[0012]
【実施例】以下、本発明を実施例に基づいてさらに詳細
に説明するが、本発明は下記実施例に何ら限定されるも
のではなく、その要旨を変更しない範囲において適宜変
更して実施することが可能なものである。EXAMPLES The present invention will be described in more detail based on the following examples, but the invention is not intended to be limited to the following examples, and various modifications may be made without departing from the scope of the invention. Is possible.
【００１３】〔正極の作製〕活物質としての二酸化マン
ガン（３７５°Ｃで熱処理した二酸化マンガン）と、導
電剤としてのアセチレンブラックと、結着剤としてのポ
リフッ化ビニリデンとを、重量比８０：１０：１０で混
合して正極合剤を調製し、この正極合剤をＮ−メチル−
２−ピロリドンに分散させてスラリーを調製し、このス
ラリーをアルミニウム箔上に塗布し、圧延し、直径２０
ｍｍの円盤状に打ち抜いた後、１５０°Ｃで２時間熱処
理して、正極を作製した。[Production of Positive Electrode] Manganese dioxide (manganese dioxide heat-treated at 375 ° C.) as an active material, acetylene black as a conductive agent, and polyvinylidene fluoride as a binder were mixed at a weight ratio of 80:10. : 10 to prepare a positive electrode mixture, and the positive electrode mixture was mixed with N-methyl-
A slurry is prepared by dispersing in 2-pyrrolidone, and the slurry is applied onto an aluminum foil and rolled to obtain a diameter of 20.
After punching out into a disk shape of mm, it was heat treated at 150 ° C. for 2 hours to produce a positive electrode.
【００１４】〔負極の作製〕金属リチウム圧延板を直径
２０ｍｍの円盤状に打ち抜いて、負極を作製した。[Production of Negative Electrode] A rolled metal lithium plate was punched into a disk shape having a diameter of 20 mm to produce a negative electrode.
【００１５】〔非水電解液の調製〕表１〜表６に組成を
示す溶媒に、トリフルオロメタンスルホン酸リチウム
（ＬｉＣＦ3 ＳＯ3 ）又はヘキサフルオロリン酸リチウ
ム（ＬｉＰＦ6 ）を１モル／リットル溶かして非水電解
液を調製した。[Preparation of Non-Aqueous Electrolyte] Lithium trifluoromethanesulfonate (LiCF 3 SO 3 ) or lithium hexafluorophosphate (LiPF 6 ) was dissolved in a solvent having a composition shown in Tables 1 to 1 mol / liter. To prepare a non-aqueous electrolyte.
【００１６】[0016]
【表１】 [Table 1]
【００１７】[0017]
【表２】 [Table 2]
【００１８】[0018]
【表３】 [Table 3]
【００１９】[0019]
【表４】 [Table 4]
【００２０】[0020]
【表５】 [Table 5]
【００２１】[0021]
【表６】 [Table 6]
【００２２】〔電池の組立〕以上の正極、負極及び非水
電解液を用いて種々の扁平型の非水電解液電池を組み立
てた（電池寸法：直径２０．０ｍｍ、厚さ２．５ｍ
ｍ）。なお、セパレータとしては、ポリプロピレン製の
微多孔膜を使用し、これに先の非水電解液を含浸させ
た。[Battery Assembly] Various flat non-aqueous electrolyte batteries were assembled using the above positive electrode, negative electrode and non-aqueous electrolyte solution (battery size: diameter 20.0 mm, thickness 2.5 m).
m). As the separator, a polypropylene microporous film was used, which was impregnated with the above non-aqueous electrolyte solution.
【００２３】〔各電池の自己放電率〕各電池の電池組立
直後の２５°Ｃでの放電容量Ｃ１及び８０°Ｃで二箇月
保存した後の２５°Ｃでの放電容量Ｃ２を求めて、各電
池の保存後の自己放電率を、下式により算出した。放電
容量Ｃ１、Ｃ２は、全て１ｋΩの定抵抗で放電して求め
たものである。結果を先の表１〜表６に示す。なお、表
中、ＥＣはエチレンカーボネートを、ＰＣはプロピレン
カーボネートを、ＢＣは、ブチレンカーボネートを、ま
たＤＭＥは１，２−ジメトキシエタンを、それぞれ表
す。[Self-Discharge Rate of Each Battery] The discharge capacity C1 of each battery immediately after assembling the battery at 25 ° C. and the discharge capacity C2 at 25 ° C. after storing at 80 ° C. for two months were obtained, and The self-discharge rate after storage of the battery was calculated by the following formula. The discharge capacities C1 and C2 are all obtained by discharging with a constant resistance of 1 kΩ. The results are shown in Tables 1 to 6 above. In the table, EC represents ethylene carbonate, PC represents propylene carbonate, BC represents butylene carbonate, and DME represents 1,2-dimethoxyethane.
【００２４】 自己放電率（％）＝（１−Ｃ２／Ｃ１）×１００Self-discharge rate (%) = (1−C2 / C1) × 100
【００２５】表１〜表５に示すように、特定の添加剤を
含有する非水電解液（添加剤含有率はいずれも５体積
％）を使用した本発明電池は、添加剤を含有しない溶媒
及び溶質が同じ非水電解液を使用した比較電池に比べ
て、自己放電率が低い。このことから、非水電解液に特
定の添加剤を含有させることにより、保存特性に優れた
非水電解液電池が得られることが分かる。As shown in Tables 1 to 5, the battery of the present invention using a non-aqueous electrolyte solution containing a specific additive (each additive content is 5% by volume) is a solvent containing no additive. In addition, the self-discharge rate is lower than that of the comparative battery using the non-aqueous electrolyte solution having the same solute. From this, it can be seen that by adding a specific additive to the non-aqueous electrolyte, a non-aqueous electrolyte battery having excellent storage characteristics can be obtained.
【００２６】また、表１中の本発明電池Ｘが、表３中の
本発明電池Ｙに比べて自己放電率が低いことから、高率
放電溶媒と１，２−ジメトキシエタンとの混合溶媒を使
用することにより、より一層保存特性に優れた非水電解
液電池が得られることが分かる。Since the battery X of the present invention in Table 1 has a lower self-discharge rate than the battery Y of the present invention in Table 3, a mixed solvent of a high rate discharge solvent and 1,2-dimethoxyethane was used. It can be seen that a non-aqueous electrolyte battery having more excellent storage characteristics can be obtained by using it.
【００２７】さらに、表６に示すように、添加剤含有率
を１〜２０体積％とした場合は、自己放電率が５％と極
めて低いのに対して、添加剤含有率がこの範囲を外れる
と自己放電率が高くなる。このことから、非水電解液の
添加剤含有率を１〜２０体積％の範囲に規制する必要が
あることが分かる。Further, as shown in Table 6, when the additive content is 1 to 20% by volume, the self-discharge rate is as low as 5%, whereas the additive content is out of this range. And the self-discharge rate becomes high. From this, it is understood that it is necessary to regulate the additive content of the non-aqueous electrolytic solution within the range of 1 to 20% by volume.
【００２８】[0028]
【発明の効果】添加剤がリチウムなどと反応して負極の
表面に被膜を形成し、この被膜が負極と非水電解液の反
応を起こりにくくするので、長期間保存した場合でも自
己放電が起こりにくい。このため、本発明電池は、保存
特性に優れる。The additive reacts with lithium or the like to form a film on the surface of the negative electrode, and this film makes it difficult for the reaction between the negative electrode and the non-aqueous electrolyte to occur, so that self-discharge occurs even when stored for a long period of time. Hateful. Therefore, the battery of the present invention has excellent storage characteristics.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 西尾 晃治 大阪府守口市京阪本通２丁目５番５号 三 洋電機株式会社内 (72)発明者 斎藤 俊彦 大阪府守口市京阪本通２丁目５番５号 三 洋電機株式会社内 ─────────────────────────────────────────────────── ─── Continuation of front page (72) Inventor Koji Nishio 2-5-5 Keihan Hondori, Moriguchi-shi, Osaka Sanyo Electric Co., Ltd. (72) Inventor Toshihiko Saito 2-chome, Keihanhondori, Moriguchi-shi, Osaka No. 5 Sanyo Electric Co., Ltd.
Claims (2)
エチレンカーボネート、プロピレンカーボネート及びブ
チレンカーボネートよりなる群から選ばれた少なくとも
一種の高誘電率溶媒を含有する溶媒にトリフルオロメタ
ンスルホン酸リチウム又はヘキサフルオロリン酸リチウ
ムを溶かしてなる非水電解液と、セパレータとを備える
非水電解液電池であって、前記非水電解液が、トリエチ
ルアミン、ｎ−ブチルアミン、アニリン、トリメチルヒ
ドロキシルアミン、１−ジメチルアミノ−２−メトキシ
エタン、アセトニトリル、アクリロニトリル、３−メト
キシプロピオニトリル、ベンゾニトリル、ニトロメタ
ン、ニトロエタン、Ｎ，Ｎ−ジメチルアセトアミド、
Ｎ，Ｎ−ジメチルホルムアミド、ホルムアミド、Ｎ−メ
チル−２−ピロリドン、Ｎ，Ｎ' −ジメチルイミダゾリ
ジノン、イソキサゾール、３，５−ジメチルイソキサゾ
ール、３−メチル−２−オキサゾリドン、１，２，３−
オキサジアゾール、Ｎ−メチルモルホリン、ジメチルス
ルフィド、エチルメチルスルフィド、２−メチルチオフ
ェン、１−ブタンチオール、ベンゼンチオール、ジメチ
ルサルフェート、ジエチルサルフェート、ジメチルサル
ファイト、ジエチルサルファイト、ブタジエンスルホ
ン、３−メチルスルホレン、１，４−チオキサン、フェ
ノキサチイン、１，４−チアジン、チオモルホリン、ピ
リジン、１，３−ジメチル−２−イミダゾリジノン、ジ
メチルスルホキシド、ジメチルスルホン、メチルエチル
スルホネート及びジメチルスルフィナイトよりなる群か
ら選ばれた少なくとも１種の添加剤を１〜２０体積％含
有することを特徴とする非水電解液電池。1. A positive electrode, a negative electrode using lithium as an active material,
Ethylene carbonate, propylene carbonate and a nonaqueous electrolytic solution obtained by dissolving lithium trifluoromethanesulfonate or lithium hexafluorophosphate in a solvent containing at least one high dielectric constant solvent selected from the group consisting of butylene carbonate, and a separator. In the non-aqueous electrolyte battery, the non-aqueous electrolyte solution is triethylamine, n-butylamine, aniline, trimethylhydroxylamine, 1-dimethylamino-2-methoxyethane, acetonitrile, acrylonitrile, 3-methoxypropionitrile. , Benzonitrile, nitromethane, nitroethane, N, N-dimethylacetamide,
N, N- dimethylformamide, formamide, N- methyl-2-pyrrolidone, N, N '- dimethyl imidazolidinone, isoxazole, 3,5-dimethyl isoxazole, 3-methyl-2-oxazolidone, 1,2, 3-
Oxadiazole, N-methylmorpholine, dimethylsulfide, ethylmethylsulfide, 2-methylthiophene, 1-butanethiol, benzenethiol, dimethylsulfate, diethylsulfate, dimethylsulfite, diethylsulfite, butadienesulfone, 3-methylsulfone From len, 1,4-thioxane, phenoxathiin, 1,4-thiazine, thiomorpholine, pyridine, 1,3-dimethyl-2-imidazolidinone, dimethyl sulfoxide, dimethyl sulfone, methyl ethyl sulfonate and dimethyl sulfinite A non-aqueous electrolyte battery containing at least one additive selected from the group consisting of 1 to 20% by volume.
シエタンを含有する請求項１記載の非水電解液電池。2. The non-aqueous electrolyte battery according to claim 1, wherein the non-aqueous electrolyte further contains 1,2-dimethoxyethane.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP7150844A JPH08321312A (en) | 1995-05-24 | 1995-05-24 | Nonaqueous electrolyte battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP7150844A JPH08321312A (en) | 1995-05-24 | 1995-05-24 | Nonaqueous electrolyte battery |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH08321312A true JPH08321312A (en) | 1996-12-03 |
Family
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Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP7150844A Pending JPH08321312A (en) | 1995-05-24 | 1995-05-24 | Nonaqueous electrolyte battery |
Country Status (1)
| Country | Link |
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| JP (1) | JPH08321312A (en) |
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