JPH01209663A - Nonaqueous secondary battery - Google Patents
Nonaqueous secondary batteryInfo
- Publication number
- JPH01209663A JPH01209663A JP63034151A JP3415188A JPH01209663A JP H01209663 A JPH01209663 A JP H01209663A JP 63034151 A JP63034151 A JP 63034151A JP 3415188 A JP3415188 A JP 3415188A JP H01209663 A JPH01209663 A JP H01209663A
- Authority
- JP
- Japan
- Prior art keywords
- lithium
- manganese dioxide
- active material
- positive electrode
- 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
- H01M4/00—Electrodes
- H01M4/02—Electrodes composed of, or comprising, active material
- H01M4/36—Selection of substances as active materials, active masses, active liquids
- H01M4/48—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
- H01M4/50—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
- H01M4/505—Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese of mixed oxides or hydroxides containing manganese for inserting or intercalating light metals, e.g. LiMn2O4 or LiMn2OxFy
-
- 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
- Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Battery Electrode And Active Subsutance (AREA)
- Secondary Cells (AREA)
Abstract
Description
【発明の詳細な説明】
Ｋｌ 産業上の利用分野
本発明はリチウム或いはリチウム合金を負極活物質とす
る非水系二次電池に係り、特に正極の改良に関するもの
である。Detailed Description of the Invention Kl Industrial Application Field The present invention relates to a non-aqueous secondary battery using lithium or a lithium alloy as a negative electrode active material, and particularly relates to improvement of the positive electrode.
（藺 従来の技術
この棟二次電池の正極活物質としては三酸化モリブデン
、五酸化バナジ９ム、チタン或いはニオブの硫化物など
が提案されているが未だ実用化には至っていない。(Background Art) Molybdenum trioxide, vanadium pentoxide, titanium, or niobium sulfide have been proposed as positive electrode active materials for secondary batteries, but they have not yet been put to practical use.
一方、非水系−次電池の正極活物質としては二酸化マン
ガン、ツク化炭素が代表的なものとして知られており、
且これらは既に実用化されている。On the other hand, manganese dioxide and carbon sulfide are known as typical positive electrode active materials for non-aqueous secondary batteries.
Moreover, these have already been put into practical use.
ここで、特に二酸化マンガンは保存性に優れ、資源的に
豊富であり且安価であるという利点を有するものである
。Here, manganese dioxide in particular has the advantages of excellent preservability, abundant resources, and low cost.
上記せる背景に鑑みて、非水系二次電池の正極活物質と
して二酸化マンガンを用いることが有益であると考えら
れるが、二酸化マンガンは可逆性に難があり充放電サイ
クル特性に問題があった。In view of the above background, it is considered to be beneficial to use manganese dioxide as a positive electrode active material for non-aqueous secondary batteries, but manganese dioxide has difficulty in reversibility and has problems in charge-discharge cycle characteristics.
ｌ／ｊ 発明が解決しようとする課題二酸化マンガン
の可逆性を改善し、二酸化マンガン−リチウム系非水二
次電池の充放電サイクル特性を向上させようとするもの
である。l/j Problem to be Solved by the Invention The present invention aims to improve the reversibility of manganese dioxide and improve the charge/discharge cycle characteristics of a manganese dioxide-lithium based non-aqueous secondary battery.
に）課題を解決するための手段
本発明はＬｉｚＭｎＯｘを正極活物質として用いること
を要旨とするものである。B) Means for Solving the Problems The gist of the present invention is to use LizMnOx as a positive electrode active material.
又、Ｌｉ２ＭｎＯ３は二酸化・マンガンとリチウム塩と
の混合物を３００〜４３０℃の温度で熱処理して得るこ
とが有益である。It is also advantageous to obtain Li2MnO3 by heat treating a mixture of manganese dioxide and lithium salt at a temperature of 300 to 430C.
Ｇｔ４作用
本件出願人が特願昭６１−２５８９４０号で提案したよ
うに、正極として二酸化マンガン活物質にＬｉ２ＭｎＯ
３を添加したものを用いると充放電サイクル特性が向上
するう
ここで正極活物質としてＬｉ２ＭｎＯｓのみを用いた場
合には放電容量の減少が生じることから、深い深度での
充放電サイクル特性ではＬｉ２ＭｎＯ３を含有した二酸
化マンガンの場合味り劣る。Gt4 action As proposed by the applicant in Japanese Patent Application No. 61-258940, Li2MnO is added to the manganese dioxide active material as a positive electrode.
However, if only Li2MnOs is used as the positive electrode active material, the discharge capacity will decrease. The taste is inferior when it contains manganese dioxide.
しかし、浅い深度の充放゛醒すイクル特性においては、
Ｌｉ２ＭｎＯ３単独の方が可逆性にすぐれていることか
ら、Ｌｉ２ＭｎＯ３を含有した二酸化マンガンの場合に
比して特性の向上が見られる。However, in the charging and awakening cycle characteristics at shallow depths,
Since Li2MnO3 alone has better reversibility, the properties are improved compared to the case of manganese dioxide containing Li2MnO3.
又、Ｌｉ２ＭｎＯ３は二酸化マンガンとリチウム塩との
混合物を３００〜４３０℃の温度で熱処理することによ
り得られるので、この方法によれば、Ｌｉ２ＭｎＯ３の
生成と二酸化マンガン中に含まれる水分除去のための熱
処理とを同時に行い得るという利点があるっ
尚、このＬｉ２ＭｎＯ３の生成時における熱処理によっ
て、二酸化マンガン中の水分のうち結合水まで除去する
ことを目的とするならば、熱処理温度としては５５０〜
４３０℃の範囲が特に好ましい。Furthermore, since Li2MnO3 can be obtained by heat-treating a mixture of manganese dioxide and lithium salt at a temperature of 300 to 430°C, according to this method, heat treatment for producing Li2MnO3 and removing water contained in manganese dioxide is possible. However, if the purpose is to remove even the bound water from the moisture in manganese dioxide by the heat treatment during the formation of Li2MnO3, the heat treatment temperature should be 550~550℃.
A range of 430°C is particularly preferred.
Ｌｉ２ＭｎＯ３を作成する時の二酸化マンガンとリチウ
ム塩の混合比については、化学式から考えられるように
Ｍｎ ：Ｌｉ＝ １ ： ２ （モル比）で混合して熱
処理すれば良い。Regarding the mixing ratio of manganese dioxide and lithium salt when creating Li2MnO3, as can be seen from the chemical formula, the mixture may be Mn:Li=1:2 (molar ratio) and then heat treated.
（へ）実施例 以ド本発明の実施例について詳述する。(f) Example Examples of the present invention will now be described in detail.
平均粒径３０μ以ドの化学二酸化マンガン５０ノと水酸
化リチウム２８Ｆを乳鉢にて混合した後、空気中に３い
て６７５℃で２０時間熱処理する１゜この熱処理により
ＬｉｚＭｎＯｓが得られる、このようにして得られた活
物質粉末と、導電剤としてのアセチレンブラック及び結
肴剤としてのフッ素樹脂粉末を重量比で９０：６：４の
比率で混合して正極合剤とし、この正極合剤を２トン／
ｃｔで直径２０ｍに加圧成型したのち２５０℃で熱処
理して正極とする。負極は所定厚みのリチウム板を直径
２０懇に打抜いたものである。After mixing 50 grams of chemical manganese dioxide with an average particle size of 30 μ or more and 28 F of lithium hydroxide in a mortar, the mixture is heated in air at 675° C. for 20 hours. Through this heat treatment, LizMnOs is obtained. The active material powder obtained by ton/
After pressure molding to a diameter of 20 m using ct, heat treatment was performed at 250°C to obtain a positive electrode. The negative electrode was made by punching out a lithium plate with a predetermined thickness to a diameter of 20 mm.
第１図は上記せる正負極を用いて組立てた扁平型非水電
解液二次電池の半断面図を示し、（１１（２＋はステン
レス製の正負極缶であってこれらはポリプロピレン製の
絶縁バッキング（３）により隔離されている。（４）は
本発明の要旨とする正極であって正極缶（１）の内底面
に固着せる正極家電体＋５１に圧接されている。（６）
は負極であって負極缶（２）の内底面に固着せる負極集
電体（７）に圧着されている。（８）はポリプロピレン
製微孔性薄膜、よりなるセパレータであり、又電解液と
してプロピレンカーボネートとジメトキシエタンとの混
合溶媒に過塩素酸リチウムを１モル／ｅ溶解したものを
用いた。電池寸法は直径２４．Ｏｓｍ、厚み五〇閣であ
った。この本発明電池を（Ａ）とするう
比較例１
リチウム塩を添加しないことを除いて他は実施例１と同
様の比較電池（Ｂ１）を作製した。Figure 1 shows a half-sectional view of a flat non-aqueous electrolyte secondary battery assembled using the above-mentioned positive and negative electrodes. (3). (4) is the positive electrode which is the gist of the present invention, and is pressure-welded to the positive electrode home appliance +51 fixed to the inner bottom surface of the positive electrode can (1). (6)
is a negative electrode, which is crimped to a negative electrode current collector (7) fixed to the inner bottom surface of the negative electrode can (2). (8) is a separator made of a microporous thin film made of polypropylene, and the electrolyte used was one in which 1 mol/e of lithium perchlorate was dissolved in a mixed solvent of propylene carbonate and dimethoxyethane. Battery dimensions are 24mm in diameter. Osm had a thickness of 50 kaku. Comparative Example 1 This invention battery was referred to as (A). A comparative battery (B1) was prepared in the same manner as in Example 1 except that no lithium salt was added.
比較例２
実施例１と同様に二酸化マンガンに水酸化リチウムをＭ
ｎ：Ｌｉ−１：２（モル比）で添加混合するが、この混
合物を熱処理しないことを除いて実施例１と同様の比較
電池（Ｂ２）を作製した。Comparative Example 2 Lithium hydroxide was added to manganese dioxide in the same manner as in Example 1.
A comparative battery (B2) was prepared in the same manner as in Example 1 except that n:Li was added and mixed at a 1:2 (molar ratio), but this mixture was not heat-treated.
比較例３
実施例１と同様に二酸化マンガンに水酸化リチウムを添
加、混合するが混合比をＭｎ：Ｌｉ＝７０：３０とする
ことを除いて実施例１と同様の比較電池（Ｂ３）を作製
した。尚、この場合の正極は二酸化マンガンとＬｉ２Ｍ
ｎＯ３とが共存した形態となっている。Comparative Example 3 A comparative battery (B3) was prepared in the same manner as in Example 1, except that lithium hydroxide was added and mixed with manganese dioxide in the same manner as in Example 1, but the mixing ratio was Mn:Li = 70:30. did. In addition, the positive electrode in this case is manganese dioxide and Li2M
It is in a form in which nO3 coexists.
第２図はこれら電池の充放電サイクル特性図を示し、充
放電条件は電流グ３ｍＡで１時間放電し、電流３ｍＡで
充電し充電終止電圧４． ＯＶとした。FIG. 2 shows the charging/discharging cycle characteristics of these batteries, and the charging/discharging conditions were: discharging at a current of 3 mA for 1 hour, charging at a current of 3 mA, and charging end voltage at 4.5 mA. It was set as OV.
第２図より本発明電池（Ａ）はサイクル特性が改善され
ているのがわかるっ又、比較電池（Ｂ２）の特性から例
えリチウム塩を添加してもＬｉ２ＭｎＯ３の形態で正極
に存在しなければサイクル特性向上に充分な効果が得ら
れないことがわかる。From Figure 2, it can be seen that the battery of the present invention (A) has improved cycle characteristics.Also, from the characteristics of the comparative battery (B2), even if lithium salt is added, it must be present in the positive electrode in the form of Li2MnO3. It can be seen that a sufficient effect in improving cycle characteristics cannot be obtained.
更ｌζ、比較電池（Ｂ３）の特性との対比から、浅い深
度の充放電に３いてはＬｉ２ＭｎＯｘ単独の方がサイク
ル特性にすぐれることがわかる。Furthermore, from comparison with the characteristics of the comparative battery (B3), it can be seen that Li2MnOx alone has better cycle characteristics when it comes to charging and discharging at a shallow depth.
尚、本実施例のようにＬｉ２ＭｎＯ３を、二酸化マンガ
ンとリチウム塩との混合物を熱処理して得る場合におい
て、リチウム塩としては実施例で例示したものに限定さ
れず硝酸リチウムやリン酸リチウムを適用できる。In addition, when Li2MnO3 is obtained by heat treating a mixture of manganese dioxide and lithium salt as in this example, the lithium salt is not limited to those exemplified in the example, and lithium nitrate or lithium phosphate can be used. .
又、熱処理温間については３００℃以上でＬｉ２ＭｎＯ
３の生成が確認されること及び４３０℃以上では二酸化
マンガンが分解されることから、３００〜４３０℃の温
度範囲が好ましい。In addition, regarding warm heat treatment, Li2MnO
A temperature range of 300 to 430°C is preferable because the formation of No. 3 is confirmed and manganese dioxide is decomposed at temperatures above 430°C.
（ト）発明の効果
上述した如く、リチウム或いはリチウム合金を活物質と
する負極を用いた非水系二次電池において、Ｌｉ２Ｍｎ
Ｏ３を活物質とする正極を用いることにより、充放電サ
イクル特性を改善することができるものであり、その工
業的価値は極めて犬である。(g) Effects of the invention As mentioned above, in a non-aqueous secondary battery using a negative electrode containing lithium or a lithium alloy as an active material, Li2Mn
By using a positive electrode containing O3 as an active material, the charge/discharge cycle characteristics can be improved, and its industrial value is extremely high.
尚、本発明を説明するに際して、非水電解液二次電池を
例にとり説明したが、固体電解質二次電池にも適用する
ことができる。Although the present invention has been explained using a non-aqueous electrolyte secondary battery as an example, it can also be applied to a solid electrolyte secondary battery.
第１図は本発明電池の半断面図、第２図は電池の充放電
サイクル特性図である。
（１）・・・正極缶、（２）・・・負極缶、（３１・・
・絶縁バッキング、（４）・・・正極、（６）・・・負
極、（８）・・・セパレータ、（Ａ）・・・本発明電池
、（Ｂ１）（Ｂ２）（Ｂ３）・・・比較電池。FIG. 1 is a half-sectional view of the battery of the present invention, and FIG. 2 is a diagram of the charge/discharge cycle characteristics of the battery. (1)...Positive electrode can, (2)...Negative electrode can, (31...
・Insulating backing, (4)...Positive electrode, (6)...Negative electrode, (8)...Separator, (A)...Battery of the present invention, (B1) (B2) (B3)... Comparison battery.
Claims (2)
と、Ｌｉ＿２ＭｎＯ＿３を活物質とする正極とを備えた
非水系二次電池。(1) A non-aqueous secondary battery comprising a negative electrode using lithium or a lithium alloy as an active material and a positive electrode using Li_2MnO_3 as an active material.
ウム塩との混合物を３００〜４３０℃の温度で熱処理し
て得られるものである請求項１記載の非水系二次電池。(2) The non-aqueous secondary battery according to claim 1, wherein the Li_2MnO_3 is obtained by heat-treating a mixture of manganese dioxide and lithium salt at a temperature of 300 to 430°C.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63034151A JPH07107851B2 (en) | 1988-02-17 | 1988-02-17 | Non-aqueous secondary battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP63034151A JPH07107851B2 (en) | 1988-02-17 | 1988-02-17 | Non-aqueous secondary battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH01209663A true JPH01209663A (en) | 1989-08-23 |
| JPH07107851B2 JPH07107851B2 (en) | 1995-11-15 |
Family
ID=12406200
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP63034151A Expired - Lifetime JPH07107851B2 (en) | 1988-02-17 | 1988-02-17 | Non-aqueous secondary battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH07107851B2 (en) |
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| US11588143B2 (en) | 2015-09-16 | 2023-02-21 | Panasonic Intellectual Property Management Co., Ltd. | Battery |
| US10811673B2 (en) | 2015-09-16 | 2020-10-20 | Panasonic Intellectual Property Management Co., Ltd. | Battery |
| US10854876B2 (en) | 2016-11-15 | 2020-12-01 | Panasonic Intellectual Property Management Co., Ltd. | Positive electrode active material and battery using positive electrode active material |
| US10840499B2 (en) | 2016-11-15 | 2020-11-17 | Panasonic Intellectual Property Management Co., Ltd. | Positive electrode active material and battery using positive electrode active material |
| US11081687B2 (en) | 2016-12-02 | 2021-08-03 | Panasonic Intellectual Property Management Co., Ltd. | Positive-electrode active material and battery including positive-electrode active material |
| US11043661B2 (en) | 2017-01-19 | 2021-06-22 | Panasonic Intellectual Property Management Co., Ltd. | Positive electrode active material containing lithium composite oxyfluoride and organosilicon compound, and battery including positive electrode containing the positive electrode active material |
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| Publication number | Publication date |
|---|---|
| JPH07107851B2 (en) | 1995-11-15 |
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