JPH02220357A - Nonaqueous secondary battery - Google Patents
Nonaqueous secondary batteryInfo
- Publication number
- JPH02220357A JPH02220357A JP1039924A JP3992489A JPH02220357A JP H02220357 A JPH02220357 A JP H02220357A JP 1039924 A JP1039924 A JP 1039924A JP 3992489 A JP3992489 A JP 3992489A JP H02220357 A JPH02220357 A JP H02220357A
- Authority
- JP
- Japan
- Prior art keywords
- active material
- positive electrode
- li2mno3
- mno2
- manganese dioxide
- 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】
イ、 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 A. Field of Industrial Application 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 a positive electrode.
口、 従来の技術
この種二次電池の正極活物質としては二酸化モリブデン
、五酸化バナジウム、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。2. Prior Art As positive electrode active materials for this type of secondary battery, molybdenum dioxide, vanadium pentoxide, titanium or niobium sulfides have been proposed, 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、フッ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 fluoride 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.
そこで、本件出願人は二酸化マンガンとリチウム塩とを
混合熱処理して得られるところのＬｉＪｏＯ３含有二酸
化マンガンを正極活物質として用いることを提案した（
特開昭６３−１１４０６４号公報参照）、このＬｉＪｏ
Ｏｉ含有の二酸化マンガンは、熱処理しただけの二酸化
マンガンよりも可逆性に優れ、その可逆性はＬｉＪａＯ
３の含有量が多くなるほど向上するのであるが、Ｌｉ２
Ｍｏ０．の含有量が多くなると、反面、放電容量が低下
するという問題がある。Therefore, the applicant proposed the use of LiJoO3-containing manganese dioxide, which is obtained by heat-treating a mixture of manganese dioxide and lithium salt, as a positive electrode active material (
(Refer to Japanese Patent Application Laid-open No. 114064/1983), this LiJo
Oi-containing manganese dioxide has better reversibility than heat-treated manganese dioxide, and its reversibility is better than that of LiJaO.
The higher the content of Li2, the better it is.
Mo0. On the other hand, there is a problem that when the content of is increased, the discharge capacity decreases.
ハ、 発明が解決しようとする課題
本発明はＬｉ２Ｍｏ０１含有の二酸化マンガンを正極活
物質とすることを基本とし、Ｌｉ２ＭａＯ，の分布状態
の効率化を図り、以ってＬｉ、ＭａＯ，含有の二酸化マ
ンガンを正極活物質とする場合における利点を生かし、
且欠点、即ち、放電容量の低下を抑制すること目的とす
る。C. Problems to be Solved by the Invention The present invention is based on the use of manganese dioxide containing Li2Mo01 as a positive electrode active material, and aims to improve the efficiency of the distribution state of Li2MaO, so that manganese dioxide containing Li, MaO, Taking advantage of the advantages when using as a positive electrode active material,
Further, the purpose is to suppress the disadvantage, that is, the decrease in discharge capacity.
二、 課題を解決するための手段
本発明の要旨とするところは、リチウム或いはリチウム
合金を活物質とする負極と、Ｌｉ２ＭａＯ，を含有する
二酸化マンガンを活物質とする正極とを備えるものであ
って、前記ＬｉＪｎＯ＞の分布が、二酸化マンガンの粒
子内部より粒子表面の方が高密度であることを特徴とす
る非水系二次電池にある。2. Means for Solving the Problems The gist of the present invention is to provide a negative electrode using lithium or a lithium alloy as an active material, and a positive electrode using manganese dioxide containing Li2MaO as an active material. The non-aqueous secondary battery is characterized in that the distribution of the above-mentioned LiJnO> is higher on the surface of the manganese dioxide particles than on the inside of the particles.
又、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、得られた生成物とリチウム
塩とを混合してのち３００〜４３０℃の温度で熱処理す
ることを特徴とする非水系二次電池用正極活物質の製造
法にある。In addition, a mixture of manganese dioxide and lithium salt
A method for producing a positive electrode active material for a non-aqueous secondary battery, which comprises heat-treating at a temperature of 430°C, mixing the obtained product with a lithium salt, and then heat-treating at a temperature of 300 to 430°C. .
ホ、 作用
Ｌｉ２Ｍｎ０．を含有する二酸化マンガン（ＭｎＯｚ）
が、可逆性に優れている理由については、完全には解明
されていないが、大きな要因として次の２点が考えられ
ている。第１の点は読口０２粒子中にり、ＭｏＯ，の結
晶と、賛口０□の結晶とが混在することにより、結晶構
造が充放電に対する可逆性に優れた形態となることであ
り、第２の点はＬｉ２ｎ０３がＭａＯ２よりも酸化反応
に対する活性度が低いことから、充電時の電解液の分解
が抑えられることにある。E, action Li2Mn0. Manganese dioxide (MnOz) containing
However, the reason why it has excellent reversibility has not been completely elucidated, but the following two points are thought to be major factors. The first point is that in the Yomikuchi02 particles, the crystal structure of MoO and the Hyakuchiku0□ crystals coexist, resulting in a crystal structure with excellent reversibility against charging and discharging. The second point is that since Li2n03 has lower activity toward oxidation reactions than MaO2, decomposition of the electrolyte during charging is suppressed.
これら２点の理由から、ＭａＯ２に含有するＬｉＪｏ０
部と表面とで差を持たせ、電解液分解の活千度を下げる
ために表面におけるＬ１□ＭＯＯ３の密度を高めること
により、高容量で且可逆性に優れた正極活物質が得られ
、斯る正極活物質を用いることによりサイクル特性に優
れた非水系二次電池を得ることができる。For these two reasons, LiJo0 contained in MaO2
By increasing the density of L1□MOO3 on the surface to reduce the activity of electrolyte decomposition, a positive electrode active material with high capacity and excellent reversibility can be obtained. By using a positive electrode active material, a non-aqueous secondary battery with excellent cycle characteristics can be obtained.
又、Ｍｌｌｏよとリチウム塩との混合物を３００〜４３
０℃の温度で熱処理し、得られた生成物とリチウム塩と
を混合してのち３００〜４３０℃の温度で熱処理するこ
とにより、 Ｌ＋ＪｎＯ：ｓの分布がＭｏＯ□の粒子内
部より粒子表面の方が高密度であるところのＬｉ２Ｍｎ
０．含有ＭｎＯ２を容易に作成することができる。Also, a mixture of Mllo and lithium salt was added at 300 to 43
By heat-treating at a temperature of 0°C, mixing the obtained product with a lithium salt, and then heat-treating at a temperature of 300 to 430°C, the distribution of L+JnO:s becomes closer to the surface of the MoO□ particles than inside the particles. Li2Mn has a high density
0. Containing MnO2 can be easily produced.
へ、 実施例 以下本発明の実施例について詳述する。To, Example Examples of the present invention will be described in detail below.
実施例１
平均粒径３０μ以下の化学二酸化マンガン８０ｇと、水
酸化リチウム１５ｇとを乳鉢にて混合した後、空気中に
おいて３７５℃で１８時間熱処理する。ついで、この生
成１１１１０２８５ ｇと水酸化リチウム５ｇとを再度
乳鉢で混合した後、空気中において３７５℃で２時間熱
処理する。Example 1 80 g of chemical manganese dioxide having an average particle size of 30 μm or less and 15 g of lithium hydroxide are mixed in a mortar, and then heat treated in air at 375° C. for 18 hours. Next, 11110285 g of this product and 5 g of lithium hydroxide are mixed again in a mortar, and then heat treated in air at 375° C. for 2 hours.
このようにして得たＬｉ２ＭｏＯ３含有のＭｏＯ２を正
極活物質とし、導電剤としてのアセチレンブラック及び
結着剤としてのフッ素樹脂扮末を重量比で９０：６：４
の比率で混合し正極合剤とし、この正極合剤を２トン／
■工で直径２０ｍ＋ａに加圧成型したのち２５０℃で熱
処理して正極とする。The thus obtained Li2MoO3-containing MoO2 was used as a positive electrode active material, and acetylene black as a conductive agent and fluororesin powder as a binder were mixed in a weight ratio of 90:6:4.
Mix at a ratio of 2 tons to make a positive electrode mixture.
After being pressure-molded to a diameter of 20m+a in step (3), it was heat-treated at 250°C to form a positive electrode.
負極は所定厚みのリチウム板を直径２Ｃ）ｖｎに打ち抜
いたものである。The negative electrode was made by punching out a lithium plate with a predetermined thickness to a diameter of 2C)vn.
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、（１）（２）はステン
レス製の正負横笛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
に固着せる正極集電体（５）に圧接されている。（６）
は負極であって負横笛（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毫ル／、溶解したものを用
いた。電池寸法は直径２４．Ｏｍ＋、厚み３．０ｍであ
った。この本発明電池を＋Ａ）とする。Figure 1 shows a half-sectional view of a flat non-aqueous electrolyte secondary battery assembled using the above-mentioned positive and negative electrodes. Isolated by backing (3). (4) is a positive electrode which is the gist of the present invention, and is pressed into contact with a positive electrode current collector (5) fixed to the inner bottom surface of the positive electrode can (1). (6)
is a negative electrode, and is crimped to a negative electrode current collector (7) fixed to the inner bottom surface of the negative transverse flute (2). (8) is a separator made of a microporous thin film made of polypropylene, and the electrolyte used is one liter/liter of lithium perchlorate dissolved in a mixed solvent of propylene carbonate and dimethoxyethane. Battery dimensions are 24mm in diameter. Om+, thickness 3.0m. This invention battery is designated as +A).
比較例１
特開昭６３−１１４０６４号公報に示されているように
、化学二酸化マンガン８０ｇと水酸化リチウム２０ｇと
を乳鉢で混合した後、空気中において３７５℃で２０時
間熱処理して得られるところのＬｉ２１１ａＯ，含有Ｍ
ｌｌＯ□を正極活物質とし、その池は実施例１と同様の
比較電池〈Ｂ、）を作製した。Comparative Example 1 As shown in JP-A No. 63-114064, 80 g of chemical manganese dioxide and 20 g of lithium hydroxide are mixed in a mortar and then heat treated in air at 375° C. for 20 hours. Li211aO, containing M
A comparative battery (B) was prepared using llO□ as the positive electrode active material and having the same pond as in Example 1.
比較例２
化学二酸化マンガン８０ｇのみを空気中において３７５
℃で２０時間熱処理して得た熱処理Ｍｏｂ。Comparative Example 2 Only 80g of chemical manganese dioxide was 375% in air.
Heat treated Mob obtained by heat treatment at ℃ for 20 hours.
を正極活物質とし、その他は実施例１と同様の比較電池
（Ｂ２）を作製した。A comparative battery (B2) was prepared in the same manner as in Example 1 except that the positive electrode active material was used as the positive electrode active material.
実施例１と比較例１で得たＬｉ２Ｍ１ｌＯ１含有のＭｎ
Ｏ２の獅町禮粒子表面におけるＬｉとＭｎのモル比をオ
ージェ電子分光法により分析した結果、実施例１のもの
はＬｉ：Ｍｎ＝２：１であり、比較例１のものはＬｉ
：Ｍｎ＝１ ： １であった。又、それぞれのＬｉ２０
Ｏ１含有ＭｏＯ□の全Ｌｉ量と全Ｍｎ量を、原子吸光法
により分析した結果、いずれもしｉ ：Ｍｎ＝１ ：
１であった。Li2M11O1-containing Mn obtained in Example 1 and Comparative Example 1
As a result of analyzing the molar ratio of Li and Mn on the surface of O2 Shimachi Rei particles by Auger electron spectroscopy, it was found that in Example 1, Li:Mn = 2:1, and in Comparative Example 1, Li:Mn was 2:1.
:Mn=1:1. Also, each Li20
As a result of analyzing the total Li content and total Mn content of O1-containing MoO□ by atomic absorption spectrometry, both i :Mn=1 :
It was 1.
このことから、実施例１におけるＬｉＪｏＯｉ含有Ｍ１
１０２は、Ｌｉ２ＭｎＯ３の分布がＭｏＯ□の粒子内部
より粒子表面の方が高密度となっているものであること
がわかる。From this, LiJoOi-containing M1 in Example 1
It can be seen that in No. 102, the distribution of Li2MnO3 is denser on the particle surface than inside the MoO□ particle.
第２図は本発明電池＋Ａ）と、比較電池＋［１１） （
［１□）の充放電サイクル特性図を示す。尚、充放電条
件は電流３ｍＡで４時間放電し、電流３ｍＡで充電し、
充電終止電圧４．０■とした。Figure 2 shows the present invention battery +A) and the comparison battery +[11) (
The charge/discharge cycle characteristic diagram of [1□] is shown. The charging and discharging conditions were: discharging at a current of 3 mA for 4 hours, charging at a current of 3 mA,
The charging end voltage was set to 4.0■.
第２図から、Ｌｉ２Ｍｎ０．含有菖口０２を正極活物質
とした電池（Ａｌｔｅｌｌは電池（Ｂ２）よりサイクル
特性が向上しているのがわかる。更に、電池（Ａ＋の方
が電池（Ｂ、）よりサイクル特性が優れているのがわか
るが、この理由は前述したようにＬｉ２Ｍｏ０１の分布
状態の差に起因する。From FIG. 2, it can be seen that Li2Mn0. It can be seen that the battery (Altell) using the containing irises 02 as the positive electrode active material has improved cycle characteristics than the battery (B2).Furthermore, the battery (A+) has better cycle characteristics than the battery (B,). The reason for this is, as described above, the difference in the distribution state of Li2Mo01.
でボした水１１１！２（乙すナワム（こ眠疋ごｒｔｖ、
＋暇すナウムやリン酸リチウム等も適用しうる。Deborashita Mizu 111! 2
+Hyakusunaum, lithium phosphate, etc. can also be applied.
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
する負極と、ＬｉＪｏ０３を含有する二酸化マンガンを
活物質とする正極とを備えた非水系二次電池において、
Ｌｉ２１ａＯｓの分布が、二酸化マンガンの粒子内部よ
り粒子表面の方が高密度であるＬｉ２Ｍｎ０．含有二酸
化マンガンを正極活物質とすることにより、放電容量の
低下が抑制でき、充放電サイクル特性を改善しうるちの
であり、その工業的価値は極めて大である。G. Effects of the invention As described above, in a non-aqueous secondary battery equipped with a negative electrode using lithium or a lithium alloy as an active material and a positive electrode using manganese dioxide containing LiJo03 as an active material,
The Li2Mn0. By using manganese dioxide as a positive electrode active material, it is possible to suppress a decrease in discharge capacity and improve charge/discharge cycle characteristics, and its industrial value is extremely large.
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）・・・負横笛、（３）・・
・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
、＋８１） （８２）・・・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 transverse flute, (3)...
- Insulating backing, (4)... Positive electrode, (6)... Negative electrode, (8)... Separator, (A)... Present invention battery, +81) (82)... Comparative battery.
Claims (2)
と、Ｌｉ＿２ＭｎＯ＿３を含有する二酸化マンガンを活
物質とする正極とを備えるものであって、前記Ｌｉ＿２
ＭｎＯ＿３の分布が、二酸化マンガンの粒子内部より粒
子表面の方が高密度であることを特徴とする非水系二次
電池。(1) A negative electrode using lithium or a lithium alloy as an active material, and a positive electrode using manganese dioxide containing Li_2MnO_3 as an active material, wherein the Li_2
A non-aqueous secondary battery characterized in that the distribution of MnO_3 is denser on the surface of manganese dioxide particles than inside the particles.
〜４３０℃の温度で熱処理し、得られた生成物とリチウ
ム塩とを混合してのち３００〜４３０℃の温度で熱処理
することを特徴とする非水系二次電池用正極活物質の製
造法。(2) 300% of a mixture of manganese dioxide and lithium salt
A method for producing a positive electrode active material for a non-aqueous secondary battery, which comprises performing a heat treatment at a temperature of -430C, mixing the obtained product and a lithium salt, and then heat-treating the mixture at a temperature of 300-430C.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1039924A JP2692932B2 (en) | 1989-02-20 | 1989-02-20 | Non-aqueous secondary battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1039924A JP2692932B2 (en) | 1989-02-20 | 1989-02-20 | Non-aqueous secondary battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH02220357A true JPH02220357A (en) | 1990-09-03 |
| JP2692932B2 JP2692932B2 (en) | 1997-12-17 |
Family
ID=12566484
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP1039924A Expired - Fee Related JP2692932B2 (en) | 1989-02-20 | 1989-02-20 | Non-aqueous secondary battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2692932B2 (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0589294A1 (en) * | 1992-09-25 | 1994-03-30 | Sanyo Electric Co., Ltd. | Nonaqueous secondary battery |
| JP2008288213A (en) * | 2008-07-14 | 2008-11-27 | Panasonic Corp | Positive electrode active material for non-aqueous electrolyte secondary battery and non-aqueous electrolyte secondary battery |
| JP2014525130A (en) * | 2011-09-20 | 2014-09-25 | エルジー・ケム・リミテッド | High capacity positive electrode active material and lithium secondary battery including the same |
| WO2025243829A1 (en) * | 2024-05-23 | 2025-11-27 | パナソニックＩｐマネジメント株式会社 | Lithium secondary battery and method for manufacturing same |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS55100224A (en) * | 1978-09-29 | 1980-07-31 | Union Carbide Corp | Mn02 derived from lim204 |
| JPS63114064A (en) * | 1986-10-30 | 1988-05-18 | Sanyo Electric Co Ltd | Nonaqueous secondary battery |
-
1989
- 1989-02-20 JP JP1039924A patent/JP2692932B2/en not_active Expired - Fee Related
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS55100224A (en) * | 1978-09-29 | 1980-07-31 | Union Carbide Corp | Mn02 derived from lim204 |
| JPS63114064A (en) * | 1986-10-30 | 1988-05-18 | Sanyo Electric Co Ltd | Nonaqueous secondary battery |
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP0589294A1 (en) * | 1992-09-25 | 1994-03-30 | Sanyo Electric Co., Ltd. | Nonaqueous secondary battery |
| JP2008288213A (en) * | 2008-07-14 | 2008-11-27 | Panasonic Corp | Positive electrode active material for non-aqueous electrolyte secondary battery and non-aqueous electrolyte secondary battery |
| JP2014525130A (en) * | 2011-09-20 | 2014-09-25 | エルジー・ケム・リミテッド | High capacity positive electrode active material and lithium secondary battery including the same |
| US9698413B2 (en) | 2011-09-20 | 2017-07-04 | Lg Chem, Ltd. | High-capacity cathode active material and lithium secondary battery including the same |
| WO2025243829A1 (en) * | 2024-05-23 | 2025-11-27 | パナソニックＩｐマネジメント株式会社 | Lithium secondary battery and method for manufacturing same |
Also Published As
| Publication number | Publication date |
|---|---|
| JP2692932B2 (en) | 1997-12-17 |
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