JPS61168870A - Metal-hydrogen alkaline storage battery - Google Patents
Metal-hydrogen alkaline storage batteryInfo
- Publication number
- JPS61168870A JPS61168870A JP60007740A JP774085A JPS61168870A JP S61168870 A JPS61168870 A JP S61168870A JP 60007740 A JP60007740 A JP 60007740A JP 774085 A JP774085 A JP 774085A JP S61168870 A JPS61168870 A JP S61168870A
- Authority
- JP
- Japan
- Prior art keywords
- alloy
- hydrogen
- electrode
- powder
- hydrogen storage
- 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
-
- 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
- H01M4/38—Selection of substances as active materials, active masses, active liquids of elements or alloys
- H01M4/383—Hydrogen absorbing alloys
-
- 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)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
Abstract
Description
【発明の詳細な説明】
（イ）産業上の利用分野
本発明は水素吸蔵合金を負極に用いる金属−水素アルカ
リ蓄電池に関し、特に高エネルギー密度で且つ長寿命に
改良された水素吸蔵合金に関する。DETAILED DESCRIPTION OF THE INVENTION (a) Industrial Application Field The present invention relates to a metal-hydrogen alkaline storage battery using a hydrogen storage alloy as a negative electrode, and particularly to a hydrogen storage alloy that has been improved to have a high energy density and a long life.
−従来の技術
従来からよく用いられる蓄電池としては鉛電池及びニッ
ケルーカドミウム電池があるが、近年これら電池より軽
量で且つ高容量となる可能性があるということで、特に
低圧に於いて負極活物質である水素を可逆的に吸蔵及び
放出することのできる水素吸蔵合金を備えた電極を負極
に用い、水酸化ニッケルなどの金属酸化物を正極活物質
とする電極を正極に用いた金属−水素アルカリ蓄電池が
注目されている。- Conventional technology Traditionally commonly used storage batteries include lead batteries and nickel-cadmium batteries, but in recent years, negative electrode active materials have been developed which have the potential to be lighter and have higher capacity than these batteries, especially at low pressure. A metal-hydrogen-alkali metal-hydrogen alkali metal-hydrogen alkali metal-hydrogen alkali metal-hydrogen-alkali material uses an electrode equipped with a hydrogen storage alloy that can reversibly absorb and release hydrogen as the negative electrode, and an electrode with a metal oxide such as nickel hydroxide as the positive electrode active material. Storage batteries are attracting attention.
一般にこの種蓄電池に用いられる水素吸蔵合金を備えた
水素吸蔵電極は特公昭５Ｂ−４６８２７号公報に於いて
提案されているように水素を吸蔵する合金粉末と水素を
吸蔵しない合金粉末との混合物を焼結して焼結多孔体を
作製し、これを水素吸蔵電極とする方法、あるいは特開
昭５３−１０３５４１号公報に於いて提案されているよ
うに水素を吸蔵する合金粉末とアセチレンブラック及び
電極支持体とを耐電解液性の粒子状結着剤により相互に
結合させて水素吸蔵電極とする方法によりて作製されて
おり、これら電極に用いる水素吸蔵合金の一つに特開昭
５１−１５９５４号公報に記載されるようなランタンな
どの希土類元素とコバルトからなる一般式ＡＣｏｓ（Ａ
は希土類元素）であられされる合金がある。しかしなが
ら、このＡＣｏｓ であられされる合金を備えた水素
吸蔵電極は、電極容量を規定する水素吸蔵歇及び充放電
によるサイクル寿命も充分満足できるものとは言えなか
った。Hydrogen storage electrodes equipped with hydrogen storage alloys that are generally used in this type of storage battery are made by using a mixture of alloy powders that store hydrogen and alloy powders that do not store hydrogen, as proposed in Japanese Patent Publication No. 5B-46827. A method of producing a sintered porous body by sintering and using it as a hydrogen storage electrode, or a method of using an alloy powder that stores hydrogen, acetylene black, and an electrode as proposed in JP-A-53-103541. Hydrogen storage electrodes are manufactured by bonding the support and the support using a particulate binder that is resistant to electrolyte to form hydrogen storage electrodes. The general formula ACos (A
There are alloys made of rare earth elements). However, the hydrogen storage electrode equipped with the alloy made of ACos cannot be said to be fully satisfactory in terms of hydrogen storage intermittent and charging/discharging cycle life, which define the electrode capacity.
Ｇｌ→ 発明が解決しようとする問題点本発明は一般式
ＡＣｏｓ（Ａは少な（とも一種の希土類元素）であられ
される合金をベースとして他の元素を含有させてなる合
金を負極に用いることにより、負極の水素吸蔵量の増加
やサイクル寿命の向上をはかろうとするものである。Gl→ Problems to be Solved by the Invention The present invention is based on an alloy with the general formula ACos (where A is a small amount (at least one kind of rare earth element)), and by using an alloy containing other elements as a negative electrode. This is an attempt to increase the hydrogen storage capacity of the negative electrode and improve its cycle life.
に）問題点を解決するための手段
本発明の金属−水素アルカリ蓄電池は、一般式ＡＣｏｓ
（Ａは少なくとも一種の希土類元素）からなる希土類元
素−コバルト合金をベースとし、該合金ニＡＩ！、Ｓ
ｔ、 Ｔｉ、 Ｖ、 Ｃｒ、 Ｍｎ、 Ｎｉ１Ｆｅ、
Ｃｕ１Ｚｎ、 Ｙ、 Ｚ ｒ、 Ｎｂ、 Ｍｏ、 Ｈｆ
、 Ｔａ及びアルカリ土類金属から選ばれる少な（とも
一種の元素を含有させたＣａＣｕ５構造の結晶構造を有
する合金を備えた負極を用いたものである。2) Means for Solving the Problems The metal-hydrogen alkaline storage battery of the present invention has the general formula ACos
(A is at least one rare earth element), and the alloy is based on a rare earth element-cobalt alloy consisting of AI! , S
t, Ti, V, Cr, Mn, Ni1Fe,
Cu1Zn, Y, Zr, Nb, Mo, Hf
, a negative electrode comprising an alloy having a CaCu5 crystal structure containing a small amount of one element selected from Ta and alkaline earth metals.
（ホ）作用
負極の水素吸蔵合金として希土類元素−コバルト合金を
ベースとし、これに前記元素の少なくとも一種を含有さ
せたＣａＣｕ５構造の結晶構造を有する合金を用いると
、負極の水素吸蔵電極の寿命が伸び容量が向上する。(e) If an alloy having a CaCu5 crystal structure based on a rare earth element-cobalt alloy and containing at least one of the above elements is used as the hydrogen storage alloy of the working negative electrode, the life of the hydrogen storage electrode of the negative electrode can be increased. Improves elongation capacity.
（ハ）実施例
市販のランタン及びコバルトを組成比でＬａ二Ｃｏ、＝
に５になるように混合し、アーク溶解炉に入れて加熱、
溶解して合金化した後粉砕してＬｘＣｏｓ粉末を得た。(c) Example Composition ratio of commercially available lanthanum and cobalt: La2Co, =
5, put it in an arc melting furnace and heat it.
After melting and alloying, it was pulverized to obtain LxCos powder.
また、ランタン、コバルト、アルミニウムを組成比でＬ
＠：Ｃｏ ：ＡＩ！−１： ４．８ ：０．２になるよ
う混合し、同様にして加熱、溶解番こよって合金化した
後粉砕を行ない、結晶構造がＣａＣｕ５構造をとるＬａ
Ｃｏ４．ＢＡＩ！Ｑ、２粉末を得ると共に、前記混合、
合金化及び粉砕という操作を行なって、結晶構造がＣ１
Ｃｕ５構造をとるＬｌ、９ＴｉＯ，ｌＣｏ４．８ＡＩ！
０．２粉末、ＬａＣｏ４．８Ｍｎ０，２粉末、ＬａＯ，
９ＴｉＱ、ｌＣｏ４．９Ｍｎ０．２粉末、Ｌａ００９Ｔ
ｉ□、ｌＣｏ５粉末、ＣｅＣｏ５粉末、ＣｅＣｏ４．８
ＡＩ！０．２粉末、ＣｅＱ、９ＴｉＯ，ｌＣｏ４．８Ａ
／Ｑ、２粉末及びＣｅＱ、９ＴｉαｌＣｏ５粉末を得た
。In addition, the composition ratio of lanthanum, cobalt, and aluminum is L.
@:Co:AI! -1:4.8:0.2, heated and melted in the same manner to form an alloy, and then crushed to obtain La with a crystal structure of CaCu5.
Co4. BAI! Q. Obtain the two powders and the mixing,
Through the operations of alloying and pulverization, the crystal structure changes to C1.
Ll with Cu5 structure, 9TiO, lCo4.8AI!
0.2 powder, LaCo4.8Mn0,2 powder, LaO,
9TiQ, lCo4.9Mn0.2 powder, La009T
i□, lCo5 powder, CeCo5 powder, CeCo4.8
AI! 0.2 powder, CeQ, 9TiO, lCo4.8A
/Q, 2 powder and CeQ, 9TiαlCo5 powder were obtained.
こうして得られた各種水種吸蔵合金粉末８０重置％、導
電材としてのアセチレンブラッ９１０重量％及び結着剤
としてのフッ素樹脂粉末１０重量％を混合機で均一に混
合すると共にフッ素樹脂を繊維化する。そして得られた
混線物をニッケル金網で包み込み３ｔｏｎ／ｄ で加圧
成型することにより、外面がニッケル金網で覆われた直
径２ｔｘ、厚み１．２ ｗｍの円形の水素吸蔵電極を種
々作製した。80% by weight of the various water type storage alloy powders thus obtained, 910% by weight of acetylene black as a conductive material, and 10% by weight of fluororesin powder as a binder are uniformly mixed in a mixer, and the fluororesin is made into fibers. do. The resulting mixed material was wrapped in a nickel wire mesh and press-molded at 3 tons/d2 to produce various circular hydrogen storage electrodes with a diameter of 2tx and a thickness of 1.2wm, the outer surface of which was covered with a nickel wire mesh.
上記外面がニッケル金網で覆われた構造の水素吸蔵電極
は、充電時に電極中の水素吸蔵合金が水素を吸蔵すると
共に水素ガスを発生して生じる電極の膨張を前記ニッケ
ル金網にょつて機械的に抑え、この電極の膨張による電
極の機械的強度の劣化及びそれに伴う水素吸蔵合金の脱
落が抑えられて、充放電サイクルによる性能の早期低下
を防止する。The hydrogen storage electrode whose outer surface is covered with a nickel wire mesh mechanically suppresses expansion of the electrode caused by the hydrogen storage alloy in the electrode absorbing hydrogen and generating hydrogen gas during charging. , the deterioration of the mechanical strength of the electrode due to the expansion of the electrode and the resulting drop-off of the hydrogen storage alloy are suppressed, thereby preventing early deterioration of performance due to charge/discharge cycles.
尚、これら水素吸蔵合金番ご用いた合金粉末は約１．５
ｆであり、１００〜３５０ｍＡＨに相画する容量を有す
る。In addition, the alloy powder used for these hydrogen storage alloy numbers is approximately 1.5
f, and has a capacity ranging from 100 to 350 mAH.
次いで、上記水素吸蔵電極を理論容量が６００ｍＡＨの
焼結式ニッケル正極と組み合わせ電解液に水酸化カリウ
ム水溶液を用いて密閉型ニッケルー水素アルカリ蓄電池
を作製し、負極に水素吸蔵材として用いた合金粉末の種
類によってこれら電池を第１表に示す様に電池Ａ乃至Ｊ
とする。またこれら電池を０．１０電流で１６時間充電
し、０．２０電流で放電して電池電圧が１．Ｏｖになっ
た時点で放電停止するサイクル条件で充放電を繰り返し
行なったときのサイクル特性を図面番こ、放電容置を第
１表に夫々示す。尚図面は各電池の初期容量を１００と
して示している。Next, a sealed nickel-hydrogen alkaline storage battery was fabricated by combining the hydrogen storage electrode with a sintered nickel positive electrode with a theoretical capacity of 600 mAH and using an aqueous potassium hydroxide solution as the electrolyte, and an alloy powder used as the hydrogen storage material for the negative electrode. Depending on the type, these batteries are listed as batteries A to J as shown in Table 1.
shall be. Also, these batteries were charged at 0.10 current for 16 hours and discharged at 0.20 current until the battery voltage was 1. The cycle characteristics when charging and discharging were repeatedly performed under cycle conditions in which the discharge was stopped when the battery reached Ov are shown in the drawing number and the discharge container in Table 1, respectively. The drawings show the initial capacity of each battery as 100.
ｌｉ表
第１表から明らかなようＧζ負極にＬ＊Ｃｏ ５、Ｃｅ
Ｃｏ５を用いた電池Ａ及びＧに比較して、これら負極に
用いた水素吸蔵合金をベースとして各種元素を含有させ
た合金を負極番こ用いた電池は何れも放電容量が増加し
ており、また図面から明らかなようにサイクル特性に関
しては電池Ｃ，Ｅ、 Ｆ、 Ｉ、 Ｊが良好な結果を示
している。これらの結果より放電容量を増大するために
はＡＩ！またはＭｎを合金に含有させることが効果的で
あり、サイクル特性を改善するためにはＴｉを合金に含
有させることが効果的であると推測できる。As is clear from Table 1, L*Co 5, Ce is added to the Gζ negative electrode.
Compared to Batteries A and G that used Co5, all of the batteries that used alloys containing various elements based on the hydrogen storage alloy used for the negative electrode had an increased discharge capacity, and As is clear from the drawings, batteries C, E, F, I, and J show good results in terms of cycle characteristics. From these results, in order to increase the discharge capacity, AI! Alternatively, it can be assumed that it is effective to include Mn in the alloy, and it is effective to include Ti in the alloy in order to improve the cycle characteristics.
同様にして負極に用いる水素吸蔵合金の組成をｔａ（：
Ｏ５をベースとし含有させる元素を種々変化させて電池
を作製し、この電池の放電容量を測定した。この結果を
負極に用いた水素吸蔵合金に対応させて第２表に示す。Similarly, the composition of the hydrogen storage alloy used for the negative electrode was changed to ta(:
Batteries were prepared using O5 as a base with various elements contained therein, and the discharge capacity of these batteries was measured. The results are shown in Table 2 in correspondence with the hydrogen storage alloy used for the negative electrode.
以下余白
第２表
また、同様にしてｔ、ａｃｏｓをベースとし含有する元
素を種々変化させた合金を負極に用いた電池を作製し、
この電池を前述のサイクル条件で充放電を繰り返し、１
０サイクル毎に容置測定を行ない放電容量が初期容量の
５０％を切った時点でサイクルを終了することによって
サイクル寿命を測定した。この結果を第３表に示す。Below is Table 2 in the margin.Also, in the same way, batteries using t, acos-based alloys with various changes in the contained elements were used as negative electrodes,
This battery was repeatedly charged and discharged under the above-mentioned cycle conditions, and
The cycle life was measured by carrying out a container measurement every 0 cycles and terminating the cycle when the discharge capacity became less than 50% of the initial capacity. The results are shown in Table 3.
第３表
このように負極の水素吸蔵合金にＡＣｏｓ （Ａは少な
くとも一種の希土類元素）で示される合金をベースとし
て各種元素を含有させたＣａＣｕ５構造の結晶構造を有
する合金を用いることにより放電容量やサイクル特性が
向上する。以上の実施例では希土類元素としてＬｌ及び
Ｃｅを示したが、その他Ｐ ｒ、 Ｎｄ、 Ｓｍ、 Ｇ
ｄの様な希土類元素を用いても同様な効果がみられ、合
金中の希土類元素を２種以上としても同様な効果がみら
れる。第４表及び第５表に夫々水素吸蔵合金に含有され
る希土類元素としてＰｒ、 Ｎｄ、 Ｓｍ、 Ｇｄを用
いた場合及び複数種の希土類元素を含有させた場合につ
いてのサイクル寿命と放電容量を示す。Table 3 As shown in Table 3, by using an alloy with a CaCu5 crystal structure containing various elements based on an alloy represented by ACos (A is at least one rare earth element) as a hydrogen storage alloy for the negative electrode, the discharge capacity can be improved. Improves cycle characteristics. In the above examples, Ll and Ce were shown as rare earth elements, but other elements such as Pr, Nd, Sm, and G
A similar effect can be seen even if a rare earth element such as d is used, and a similar effect can be seen even if two or more kinds of rare earth elements are used in the alloy. Tables 4 and 5 show the cycle life and discharge capacity when Pr, Nd, Sm, and Gd are used as rare earth elements contained in the hydrogen storage alloy, and when multiple types of rare earth elements are contained, respectively. .
以下余白
第４表
第５表
（ト）発明の効果
本発明の金属−水素アルカリ蓄電池は、希土類元素−コ
バルト合金にＡＩ！、５ｉＳＴｉ、Ｖ、Ｃｒ、Ｍｎ。Table 4 Table 5 (G) Effects of the Invention The metal-hydrogen alkaline storage battery of the present invention has a rare earth element-cobalt alloy containing AI! , 5iSTi, V, Cr, Mn.
Ｎｉ、 Ｆｅ、 Ｃｕ％Ｚｎ、 Ｙ、 Ｚｒ、 Ｎｂ、
Ｍｏ、 Ｈｆ、 Ｔａ及びアルカリ土類金属から選ば
れる少なくとも一種の元素を含有させたＣａＣｕ５構造
の結晶構造を有する合金を備えた水素吸蔵電極を負極に
用いたものであり、サイクル特性の向上や水素吸蔵量の
増大による放電容量の増加により優れた性能の蓄電池を
提供することができ、その工業的価値は極めて大である
。Ni, Fe, Cu%Zn, Y, Zr, Nb,
A hydrogen storage electrode equipped with an alloy having a CaCu5 crystal structure containing at least one element selected from Mo, Hf, Ta, and alkaline earth metals is used as the negative electrode, and it improves cycle characteristics and absorbs hydrogen. By increasing the discharge capacity due to the increase in storage capacity, a storage battery with excellent performance can be provided, and its industrial value is extremely large.
図面は各種水素吸蔵合金を負極に備えた電池のサイクル
特性を示す図面である。The drawings show the cycle characteristics of batteries with negative electrodes containing various hydrogen storage alloys.
Claims (1)
電解液とを具備する電池であって、前記負極の水素吸蔵
合金が希土類元素−コバルト合金にＡｌ、Ｓｉ、Ｔｉ、
Ｖ、Ｃｒ、Ｍｎ、Ｎｉ、Ｆｅ、Ｃｕ、Ｚｎ、Ｙ、Ｚｒ、
Ｎｂ、Ｍｏ、Ｈｆ、Ｔａ及びアルカリ土類金属から選ば
れる少なくとも一種の元素を含有させたＣａＣｕ＿５構
造の結晶構造を有する合金であることを特徴とする金属
−水素アルカリ蓄電池。(1) A battery comprising a positive electrode, a negative electrode including a hydrogen storage alloy, and an alkaline electrolyte, wherein the hydrogen storage alloy of the negative electrode includes a rare earth element-cobalt alloy, Al, Si, Ti,
V, Cr, Mn, Ni, Fe, Cu, Zn, Y, Zr,
A metal-hydrogen alkaline storage battery characterized by being an alloy having a crystal structure of CaCu_5 structure containing at least one element selected from Nb, Mo, Hf, Ta, and alkaline earth metals.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP60007740A JPS61168870A (en) | 1985-01-19 | 1985-01-19 | Metal-hydrogen alkaline storage battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP60007740A JPS61168870A (en) | 1985-01-19 | 1985-01-19 | Metal-hydrogen alkaline storage battery |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS61168870A true JPS61168870A (en) | 1986-07-30 |
Family
ID=11674096
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP60007740A Pending JPS61168870A (en) | 1985-01-19 | 1985-01-19 | Metal-hydrogen alkaline storage battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS61168870A (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS6243064A (en) * | 1985-08-20 | 1987-02-25 | Matsushita Electric Ind Co Ltd | Hydrogen occlusion alloy for alkaline storage battery |
| JPS62139258A (en) * | 1985-12-12 | 1987-06-22 | Matsushita Electric Ind Co Ltd | Electrode for storage battery |
| JPH02186559A (en) * | 1989-01-13 | 1990-07-20 | Sanyo Electric Co Ltd | Hydrogen storage alloy electrode for alkaline storage battery |
| CN107779748A (en) * | 2017-10-23 | 2018-03-09 | 南京理工大学 | Alloy material with room temperature zero thermal expansion effect and preparation method thereof |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4487817A (en) * | 1983-10-21 | 1984-12-11 | Willems Johannes J G S A | Electrochemical cell comprising stable hydride-forming material |
-
1985
- 1985-01-19 JP JP60007740A patent/JPS61168870A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US4487817A (en) * | 1983-10-21 | 1984-12-11 | Willems Johannes J G S A | Electrochemical cell comprising stable hydride-forming material |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS6243064A (en) * | 1985-08-20 | 1987-02-25 | Matsushita Electric Ind Co Ltd | Hydrogen occlusion alloy for alkaline storage battery |
| JP2666249B2 (en) * | 1985-08-20 | 1997-10-22 | 松下電器産業株式会社 | Hydrogen storage alloy for alkaline storage batteries |
| JPS62139258A (en) * | 1985-12-12 | 1987-06-22 | Matsushita Electric Ind Co Ltd | Electrode for storage battery |
| JPH0690924B2 (en) * | 1985-12-12 | 1994-11-14 | 松下電器産業株式会社 | Storage battery electrode |
| JPH02186559A (en) * | 1989-01-13 | 1990-07-20 | Sanyo Electric Co Ltd | Hydrogen storage alloy electrode for alkaline storage battery |
| CN107779748A (en) * | 2017-10-23 | 2018-03-09 | 南京理工大学 | Alloy material with room temperature zero thermal expansion effect and preparation method thereof |
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