JPS638588B2 - - Google Patents
Info
- Publication number
- JPS638588B2 JPS638588B2 JP55040025A JP4002580A JPS638588B2 JP S638588 B2 JPS638588 B2 JP S638588B2 JP 55040025 A JP55040025 A JP 55040025A JP 4002580 A JP4002580 A JP 4002580A JP S638588 B2 JPS638588 B2 JP S638588B2
- Authority
- JP
- Japan
- Prior art keywords
- lithium
- active material
- electrode active
- negative electrode
- intercalation compound
- 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.)
- Expired
Links
- GNTDGMZSJNCJKK-UHFFFAOYSA-N divanadium pentaoxide Chemical compound O=[V](=O)O[V](=O)=O GNTDGMZSJNCJKK-UHFFFAOYSA-N 0.000 claims description 28
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 25
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 22
- 239000007774 positive electrode material Substances 0.000 claims description 14
- 150000001875 compounds Chemical class 0.000 claims description 13
- 230000002687 intercalation Effects 0.000 claims description 12
- 238000009830 intercalation Methods 0.000 claims description 12
- 229910001947 lithium oxide Inorganic materials 0.000 claims description 12
- 239000004408 titanium dioxide Substances 0.000 claims description 12
- 239000005486 organic electrolyte Substances 0.000 claims description 11
- 229910052744 lithium Inorganic materials 0.000 claims description 10
- 239000007773 negative electrode material Substances 0.000 claims description 8
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 claims description 6
- 229910001416 lithium ion Inorganic materials 0.000 claims description 6
- 239000003792 electrolyte Substances 0.000 claims description 5
- 229910003002 lithium salt Inorganic materials 0.000 claims description 2
- 159000000002 lithium salts Chemical class 0.000 claims description 2
- 239000003960 organic solvent Substances 0.000 claims description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims 1
- HPGPEWYJWRWDTP-UHFFFAOYSA-N lithium peroxide Chemical compound [Li+].[Li+].[O-][O-] HPGPEWYJWRWDTP-UHFFFAOYSA-N 0.000 claims 1
- 229910052719 titanium Inorganic materials 0.000 claims 1
- 239000010936 titanium Substances 0.000 claims 1
- 238000006243 chemical reaction Methods 0.000 description 6
- 238000007599 discharging Methods 0.000 description 6
- 229910010413 TiO 2 Inorganic materials 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 239000004743 Polypropylene Substances 0.000 description 2
- 239000004809 Teflon Substances 0.000 description 2
- 229920006362 Teflon® Polymers 0.000 description 2
- 239000011230 binding agent Substances 0.000 description 2
- 229910002804 graphite Inorganic materials 0.000 description 2
- 239000010439 graphite Substances 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 238000000465 moulding Methods 0.000 description 2
- -1 polypropylene Polymers 0.000 description 2
- 229920001155 polypropylene Polymers 0.000 description 2
- 229910021607 Silver chloride Inorganic materials 0.000 description 1
- 239000011149 active material Substances 0.000 description 1
- OJIJEKBXJYRIBZ-UHFFFAOYSA-N cadmium nickel Chemical compound [Ni].[Cd] OJIJEKBXJYRIBZ-UHFFFAOYSA-N 0.000 description 1
- 239000007795 chemical reaction product Substances 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005868 electrolysis reaction Methods 0.000 description 1
- 239000008151 electrolyte solution Substances 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 239000011229 interlayer Substances 0.000 description 1
- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 1
- 230000007774 longterm Effects 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000004745 nonwoven fabric Substances 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 230000002093 peripheral effect Effects 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- RUOJZAUFBMNUDX-UHFFFAOYSA-N propylene carbonate Chemical compound CC1COC(=O)O1 RUOJZAUFBMNUDX-UHFFFAOYSA-N 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- HKZLPVFGJNLROG-UHFFFAOYSA-M silver monochloride Chemical compound [Cl-].[Ag+] HKZLPVFGJNLROG-UHFFFAOYSA-M 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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
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)
- Battery Electrode And Active Subsutance (AREA)
Description
【発明の詳細な説明】
産業上の利用分野
本発明は有機電解液二次電池に関するものであ
る。DETAILED DESCRIPTION OF THE INVENTION Field of Industrial Application The present invention relates to an organic electrolyte secondary battery.
従来技術とその問題点
有機電解液二次電池は、高エネルギー密度を得
るために負極活物質にリチウムを、正極活物質に
は高い酸化力を有するNiF2，AgClなどを用いた
ものが知られているが、いずれもサイクル寿命が
悪く、実用に耐えるものではなかつた。この原因
は正極活物質の安定性にもよるが、負極活物質の
リチウムが充放電サイクルの経過とともに変形し
て容量が低下したり、樹枝状に析出して内部短絡
ブリツジを形成することによるところが大であつ
た。さらに正極活物質とリチウムとの反応生成物
が電解液に溶解する場合には、正極活物質にも変
形を生じ、容量が低下することがあつた。Conventional technology and its problems Organic electrolyte secondary batteries are known to use lithium as the negative electrode active material and NiF 2 , AgCl, etc., which have high oxidizing power, as the positive electrode active material to obtain high energy density. However, all of them had poor cycle life and were not suitable for practical use. The cause of this depends on the stability of the positive electrode active material, but the lithium in the negative electrode active material may deform as the charge/discharge cycle progresses, resulting in a decrease in capacity, or it may precipitate into dendritic forms and form internal short bridges. It was big and warm. Furthermore, when the reaction product of the positive electrode active material and lithium is dissolved in the electrolyte, the positive electrode active material may also be deformed, resulting in a decrease in capacity.
発明の目的
本発明は上記欠点を解消するもので、有機電解
液を用いた二次電池が、アルカリ電解液のような
クリープ現象による漏液を生じないことと、水の
電気分解反応による充放電効率の低下を生じない
こととに着目し、サイクル寿命のすぐれた有機電
解液二次電池を得ることを目的とする。Purpose of the Invention The present invention solves the above-mentioned drawbacks, and aims to provide a secondary battery using an organic electrolyte that does not leak due to the creep phenomenon unlike alkaline electrolytes, and that charges and discharges due to the electrolysis reaction of water. The purpose of this invention is to obtain an organic electrolyte secondary battery with excellent cycle life, with a focus on not causing a decrease in efficiency.
発明の構成
本発明の有機電解液二次電池は、リチウム塩を
溶解した有機溶媒を電解液とし、充電状態で正極
活物質に五酸化バナジウムを、負極活物質にリチ
ウム・二酸化チタンの層間化合物を用い、放電に
よつてリチウム・二酸化チタンの層間化合物から
正極活物質へ１分子当り１個のリチウムイオンが
移動し、リチウム・五酸化バナジウムの層間化合
物が形成されるように負極容量を制限したことを
特徴とするものである。Structure of the Invention The organic electrolyte secondary battery of the present invention uses an organic solvent in which a lithium salt is dissolved as an electrolyte, and in a charged state, vanadium pentoxide is used as a positive electrode active material, and an intercalation compound of lithium and titanium dioxide is used as a negative electrode active material. The negative electrode capacity is limited so that one lithium ion per molecule moves from the lithium/titanium dioxide intercalation compound to the positive electrode active material by discharge, forming an intercalation compound of lithium/vanadium pentoxide. It is characterized by:
実施例
以下実施例により説明する。第１図は本発明の
有機電解液二次電池の半截断面図である。第１図
において、１は正極活物質で、五酸化バナジウム
（V2O5）にグラフアイトを添加してテフロンバイ
ンダーにて円板状に成形したものである。２は負
極活物質で、アナターゼ型二酸化チタン（TiO2）
にグラフアイトを添加してテフロンバインダーに
て円板状に成形してものである。３は円板状に打
ち抜いた金属リチウムで、負極活物質２の表面に
直接接触させている。４はプロピレンカーボネイ
トと1.2―ジメトシエタンとの１：１混合液に１
モル／の過塩素酸リチウムを溶解させてなる電
解液が含浸されたポリプロピレン不織布よりなる
セパレータ、５，６はそれぞれ正極および負極端
子を兼ねるステンレス製の容器と蓋で、各々の周
縁部分はポリプロピレン製のガスケツト７を介し
てかしめられている。こうして組み立てられた電
池の寸法は直径が20mm、高さが２mmで、組み立て
直後には五酸化バナジウムとリチウムとの電位差
である約3.5Vの開路電圧をすが、常温にて１週
間放置すれば次式の反応でリチウム・二酸化チタ
ンの層間化合物が形成され、約1.75Vの開路電圧
を示すようになる。Examples The following examples will be explained below. FIG. 1 is a half-cut sectional view of the organic electrolyte secondary battery of the present invention. In FIG. 1, 1 is a positive electrode active material, which is made by adding graphite to vanadium pentoxide (V 2 O 5 ) and molding it into a disc shape using a Teflon binder. 2 is the negative electrode active material, which is anatase titanium dioxide (TiO 2 )
It is made by adding graphite to it and molding it into a disk shape using a Teflon binder. 3 is a metal lithium punched into a disk shape, and is brought into direct contact with the surface of the negative electrode active material 2. 4 is 1:1 mixture of propylene carbonate and 1,2-dimethothethane.
A separator made of polypropylene non-woven fabric impregnated with an electrolytic solution made by dissolving lithium perchlorate in moles/liter; 5 and 6 are stainless steel containers and lids that also serve as positive and negative electrode terminals, respectively, and the peripheral portion of each is made of polypropylene. It is caulked through the gasket 7. The dimensions of the battery assembled in this way are 20 mm in diameter and 2 mm in height, and it has an open circuit voltage of about 3.5 V, which is the potential difference between vanadium pentoxide and lithium, immediately after assembly, but if left at room temperature for a week. An intercalation compound of lithium and titanium dioxide is formed by the following reaction, and it exhibits an open circuit voltage of approximately 1.75V.
TiO2＋Li→TiO2.Li
上記の如き構成からなる電池の起電反応は次式
で表わされる。 TiO 2 +Li→TiO 2 .Li The electromotive reaction of the battery configured as above is expressed by the following equation.
すなわち放電時には負極側のリチウム・二酸化
チタンの層間化合物から正極側の五酸化バナジウ
ムへ１分子当り１個のリチウムイオンが移動して
リチウム・五酸化バナジウムの層間化合物が形成
され、充電時には正極側のリチウム・五酸化バナ
ジウムの層間化合物から負極側の二酸化チタンへ
１分子当り１個のリチウムイオンが移動してリチ
ウム・二酸化チタンの層間化合物が形成される反
応である。このような本発明の有機電解液二次電
池の充放電反応は正、負極活物質１分当り１個の
リチウムイオンが出入りする反応で、これに伴つ
て１分子当り１個の電子が移動するものである
が、充電により回復させることができるように放
電によるリチウムイオンの移動を五酸化バナジウ
ム１分子当り１個に制限している。 In other words, during discharging, one lithium ion per molecule moves from the lithium/titanium dioxide intercalation compound on the negative electrode side to vanadium pentoxide on the positive electrode side, forming an intercalation compound of lithium/vanadium pentoxide. This is a reaction in which one lithium ion per molecule moves from the lithium/vanadium pentoxide intercalation compound to the titanium dioxide on the negative electrode side, forming an intercalation compound of lithium/titanium dioxide. The charging/discharging reaction of the organic electrolyte secondary battery of the present invention is a reaction in which one lithium ion enters and exits the positive and negative electrode active materials per minute, and accordingly, one electron moves per molecule. However, the movement of lithium ions due to discharge is limited to one per molecule of vanadium pentoxide so that it can be recovered by charging.
また本発明においては、二酸化チタンと金属リ
チウムとを電気的に接続された状態で電池内に組
み込み、自己放電反応によつてリチウム・二酸化
チタンの層間化合物を形成しているので、工業的
にも極めて有利である。 In addition, in the present invention, titanium dioxide and metallic lithium are incorporated into the battery in an electrically connected state, and an interlayer compound of lithium and titanium dioxide is formed through a self-discharge reaction, so that it can be used industrially. Extremely advantageous.
五酸化バナジウムは従来から一次電池の正極活
物質として用いられることが検討されているが、
正極活物質１分子当り２〜３個の電子の移動を伴
うのが普通であり、この場合には充電しても回復
しない。ところが研究の結果、放電量を一定限度
内すなわち正極活物質１分子当り１個の電子の移
動だけに抑えれば充電により回復させることがで
きることが判明した。実用的にはこのように放電
量を一定限度内に抑えることは難しく、過放電に
なることが予測されるので、本発明においては、
負極容量を少なくして五酸化バナジウムを過放電
させないようにした。すなわち各活物質を重量比
で五酸化バナジウム１に対し、リチウム0.038以
下、二酸化チタンを0.44以上にしてリチウム・二
酸化チタンの層間化合物が形成されるようにし、
五酸化バナジウム１分子当り１個の電子の移動だ
けに抑え、充電により容量を回復させるようにし
たことを特徴としている。 Vanadium pentoxide has been considered for use as a positive electrode active material in primary batteries, but
Usually, 2 to 3 electrons are transferred per molecule of the positive electrode active material, and in this case, it does not recover even if it is charged. However, as a result of research, it has been found that recovery can be achieved by charging if the amount of discharge is kept within a certain limit, that is, the movement of one electron per molecule of the positive electrode active material. In practice, it is difficult to suppress the discharge amount within a certain limit in this way, and overdischarge is predicted, so in the present invention,
The negative electrode capacity was reduced to prevent vanadium pentoxide from being over-discharged. That is, the weight ratio of each active material to vanadium pentoxide is 0.038 or less for lithium and 0.44 or more for titanium dioxide so that an intercalation compound of lithium and titanium dioxide is formed.
It is characterized by restricting the transfer of only one electron per molecule of vanadium pentoxide, and allowing the capacity to be restored by charging.
第２図は本発明の有機電解液二次電池を１ｍＡ
の充電電流および放電電流で充放電させた時の充
電電圧特性図である。第２図から充放電は約
1.5Vの電圧で行われ、その容量は約20ｍAhであ
ることがわかる。この本発明電池は、同一寸法の
リチウムを負極とした一次電池が約3V、60ｍAh
程度であるのに比較すれば、容量は３分の１にな
るものの、繰返し充放電を行うことができるとい
う特徴を有するものである。 Figure 2 shows the organic electrolyte secondary battery of the present invention at 1 mA.
FIG. 3 is a charging voltage characteristic diagram when charging and discharging at charging current and discharging current. From Figure 2, charging and discharging is approximately
It can be seen that the voltage is 1.5V and the capacity is about 20mAh. This invention battery has a primary battery of the same size with lithium as a negative electrode and a voltage of approximately 3V and 60mAh.
Although the capacity is only one-third of the average capacity, it has the characteristic of being able to be repeatedly charged and discharged.
発明の効果
実施例において詳述した如く、本発明の有機電
解液二次電池は、ニツケル―カドミウム二次電池
のようなアルカリ電解液を用いて二次電池に比べ
て漏液を生じることが少なく、長期間にわたる使
用に耐えるものである。Effects of the Invention As detailed in the Examples, the organic electrolyte secondary battery of the present invention has less leakage than a secondary battery using an alkaline electrolyte such as a nickel-cadmium secondary battery. , which can withstand long-term use.
第１図は本発明の有機電解液二次電池の半截断
面図、第２図は本発明電池の充放電電圧特性の一
例である。
１…正極活物質、２…負極活物質、３…金属リ
チウム、４…セパレータ、５…容器、６…蓋、７
…ガスケツト。
FIG. 1 is a half-sectional view of an organic electrolyte secondary battery of the present invention, and FIG. 2 is an example of the charging/discharging voltage characteristics of the battery of the present invention. DESCRIPTION OF SYMBOLS 1... Positive electrode active material, 2... Negative electrode active material, 3... Metal lithium, 4... Separator, 5... Container, 6... Lid, 7
...Gasket.
Claims (1)
し、充電状態で正極活物質に五酸化バナジウム
を、負極活物質に二酸化チタンと金属リチウムと
を電気的に接触させることによつて形成したリチ
ウム・二酸化チタンの層間化合物を用い、放電に
よつてリチウム・二酸化チタンの層間化合物から
正極活物質へ１分子当り１個のリチウムイオンが
移動し、リチウム・五酸化バナジウムの層間化合
物が形成されるように負極容量を制限したことを
特徴とする有機電解液二次電池。1. Lithium dioxide formed by using an organic solvent in which a lithium salt is dissolved as an electrolyte and electrically contacting vanadium pentoxide as a positive electrode active material and titanium dioxide and metallic lithium as a negative electrode active material in a charged state. A titanium intercalation compound is used in the negative electrode so that one lithium ion per molecule moves from the lithium/titanium dioxide intercalation compound to the positive electrode active material by discharge, forming an intercalation compound of lithium/vanadium pentoxide. An organic electrolyte secondary battery characterized by limited capacity.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP4002580A JPS56136462A (en) | 1980-03-27 | 1980-03-27 | Secondary battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP4002580A JPS56136462A (en) | 1980-03-27 | 1980-03-27 | Secondary battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS56136462A JPS56136462A (en) | 1981-10-24 |
| JPS638588B2 true JPS638588B2 (en) | 1988-02-23 |
Family
ID=12569355
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP4002580A Granted JPS56136462A (en) | 1980-03-27 | 1980-03-27 | Secondary battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS56136462A (en) |
Families Citing this family (9)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS57152669A (en) * | 1981-03-18 | 1982-09-21 | Sanyo Electric Co Ltd | Chargeable organic electrolyte battery |
| JPS59186274A (en) * | 1983-04-07 | 1984-10-23 | Matsushita Electric Ind Co Ltd | Manufacturing method of non-aqueous electrolyte secondary battery |
| JPS60220574A (en) * | 1984-04-17 | 1985-11-05 | Matsushita Electric Ind Co Ltd | Chargeable electrochemical apparatus |
| US7337010B2 (en) | 2004-10-29 | 2008-02-26 | Medtronic, Inc. | Medical device having lithium-ion battery |
| US9065145B2 (en) | 2004-10-29 | 2015-06-23 | Medtronic, Inc. | Lithium-ion battery |
| US8980453B2 (en) | 2008-04-30 | 2015-03-17 | Medtronic, Inc. | Formation process for lithium-ion batteries |
| US9077022B2 (en) | 2004-10-29 | 2015-07-07 | Medtronic, Inc. | Lithium-ion battery |
| US7582387B2 (en) | 2004-10-29 | 2009-09-01 | Medtronic, Inc. | Lithium-ion battery |
| JP5395426B2 (en) * | 2008-12-26 | 2014-01-22 | 日揮触媒化成株式会社 | Electrode material for lithium battery and lithium battery |
-
1980
- 1980-03-27 JP JP4002580A patent/JPS56136462A/en active Granted
Also Published As
| Publication number | Publication date |
|---|---|
| JPS56136462A (en) | 1981-10-24 |
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