JPH03126832A - Hydrogen occluding electrode for alkaline storage battery - Google Patents
Hydrogen occluding electrode for alkaline storage batteryInfo
- Publication number
- JPH03126832A JPH03126832A JP1264238A JP26423889A JPH03126832A JP H03126832 A JPH03126832 A JP H03126832A JP 1264238 A JP1264238 A JP 1264238A JP 26423889 A JP26423889 A JP 26423889A JP H03126832 A JPH03126832 A JP H03126832A
- Authority
- JP
- Japan
- Prior art keywords
- storage battery
- alkaline storage
- hydrogen storage
- cycle life
- electrode
- 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
- 239000001257 hydrogen Substances 0.000 title abstract description 25
- 229910052739 hydrogen Inorganic materials 0.000 title abstract description 25
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title abstract description 24
- 229910052721 tungsten Inorganic materials 0.000 claims abstract description 5
- 229910001122 Mischmetal Inorganic materials 0.000 claims 1
- 239000000956 alloy Substances 0.000 abstract description 30
- 229910045601 alloy Inorganic materials 0.000 abstract description 30
- 229910052804 chromium Inorganic materials 0.000 abstract description 5
- 229910052751 metal Inorganic materials 0.000 abstract 1
- 239000002184 metal Substances 0.000 abstract 1
- 150000002739 metals Chemical class 0.000 abstract 1
- 239000000203 mixture Substances 0.000 description 9
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 5
- 230000000694 effects Effects 0.000 description 4
- 239000000843 powder Substances 0.000 description 4
- 239000013078 crystal Substances 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 241000283986 Lepus Species 0.000 description 2
- 229910052793 cadmium Inorganic materials 0.000 description 2
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- KWYUFKZDYYNOTN-UHFFFAOYSA-M Potassium hydroxide Chemical compound [OH-].[K+] KWYUFKZDYYNOTN-UHFFFAOYSA-M 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 239000011230 binding agent Substances 0.000 description 1
- OJIJEKBXJYRIBZ-UHFFFAOYSA-N cadmium nickel Chemical compound [Ni].[Cd] OJIJEKBXJYRIBZ-UHFFFAOYSA-N 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 230000007797 corrosion Effects 0.000 description 1
- 238000005260 corrosion Methods 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 239000000835 fiber Substances 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 230000001771 impaired effect Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
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
- Battery Electrode And Active Subsutance (AREA)
Abstract
Description
【発明の詳細な説明】
〔産業上の利用分野〕
本発明は、アルカリ蓄電池の負極として用いられ、水素
を可逆的に吸蔵、放出する水素吸蔵合金から成るアルカ
リ蓄電池用水素吸蔵電極に関する。DETAILED DESCRIPTION OF THE INVENTION [Field of Industrial Application] The present invention relates to a hydrogen storage electrode for an alkaline storage battery, which is used as a negative electrode of an alkaline storage battery and is made of a hydrogen storage alloy that reversibly stores and releases hydrogen.
従来、各種の電気又は電子応用機器の電源としてアルカ
リ蓄電池が広く用いられている。該アルカリ蓄電池のう
ち、最も広く使用されているのは、ニッケルーカドミウ
ム蓄電池であるが、更に、高エネルギー密度を有し、無
公害の新しい二次電池として、最近、水素を可及的に吸
蔵、放出する水素吸蔵合金を負極として用いるアルカリ
蓄電池がｒＷ１発されている。この水素吸蔵合金は、カ
ドミウムと同じ取り扱いで電池の電極として構成でき、
実際の放電可能な容量密度をカドミウムよりも大きくで
きることから、高エネルギー密度で無公害のアルカリ蓄
電池として有望である。この種の水素吸蔵合金電極とし
て、ＬａＮ ｌ ｓ合金、ＬａＮ１ｔ Ｃｏ３合金、Ｌ
ａＮｉ＜、ｓ Ｈｎｏ、ｑ合金などの水素吸蔵合金を用
いたものは公知である。Conventionally, alkaline storage batteries have been widely used as power sources for various electrical or electronic applied devices. Among these alkaline storage batteries, the most widely used is the nickel-cadmium storage battery, but recently, as a new secondary battery that has high energy density and is non-polluting, it has been developed to absorb as much hydrogen as possible. , an alkaline storage battery using a releasing hydrogen storage alloy as a negative electrode has been emitted rW1. This hydrogen storage alloy can be used as a battery electrode in the same way as cadmium.
Since the actual dischargeable capacity density can be made higher than that of cadmium, it is promising as a high energy density, pollution-free alkaline storage battery. As this type of hydrogen storage alloy electrode, LaNl s alloy, LaN1tCo3 alloy, L
Those using hydrogen storage alloys such as aNi<, s Hno, and q alloys are known.
上記従来の合金を水素吸蔵合金をアルカリ蓄電池の負極
として用いた場合、サイクル寿命が短い欠点がある。When the above-mentioned conventional hydrogen storage alloy is used as a negative electrode of an alkaline storage battery, there is a drawback that the cycle life is short.
本発明は、かＮる上記従来のアルカリ蓄電池用水素吸蔵
電極を改善−し、サイクル寿命の著しく増大したアルカ
リ蓄電池用水素吸蔵電極を提供するもので、一般式Ｈｎ
Ｎｉ、 Ｃｏｂ Ｈｎｃ ＡｄＢ −（但し、）４ｎは
ミツシュメタル、ＡはＡＩ、 Ｓｉ及びＣｒから成る群
より撰ばれた少なくとも一種、ＢはＷ及びＧｅから成る
群より撰ばれた少なくとも一種、且ツ４．５≦ａ＋ｂ＋
ｃ＋ｄ＋ｅ≦５．５．０＜ｄ≦０．６ ０＜ｅ≦０．３
）で表される水素吸蔵合金から成る。The present invention improves the conventional hydrogen storage electrode for alkaline storage batteries described above and provides a hydrogen storage electrode for alkaline storage batteries with a significantly increased cycle life.
Ni, Cob Hnc AdB - (However, ) 4n is Mitsushmetal, A is AI, at least one selected from the group consisting of Si and Cr, B is at least one selected from the group consisting of W and Ge, and 4. 5≦a+b+
c+d+e≦5.5.0<d≦0.6 0<e≦0.3
) consists of a hydrogen storage alloy represented by
上記の構成の水素吸蔵合金電極をアルカリ蓄電池の負極
として用いるときは、合金腐食による特性劣化が小さく
、サイクル寿命の長いアルカリ蓄電池をもたらす。When the hydrogen storage alloy electrode having the above structure is used as a negative electrode of an alkaline storage battery, an alkaline storage battery with less characteristic deterioration due to alloy corrosion and a long cycle life is produced.
次に、本発明の実施例につき説明する。 Next, examples of the present invention will be described.
市販のＭｌ例えば、ｌａ：３０重量・％、Ｃｅ：４５重
量％、Ｎｄ：１５重量％、Ｐｒ：５：ｌｉ量％他）Ｎｉ
、Ｃ０ｌＭｎの他に、Ａ１とＷを選択し、下記第１表に
列挙する夫々の組成成分と組成比で夫々秤量、配合し、
次でアルゴンアーク溶解炉で加熱溶融して１４種類の合
金を得た。これらの合金を夫々機械的に３２μｍ以下に
粉砕し、夫々の組成成分と原子数比をもつ各種組成の１
４種類の水素吸蔵合金粉末を得た。これら１４種類の合
金粉末の夫々について、導電材としてＮ１粉を２０重量
％、結着剤としてフッ素樹脂粉末を５重量％添加し、混
合してフッ素樹脂繊維化させた後、粉砕して得られた各
混合物を、ニッケル金網上に均一な厚さに積層し、ｉｔ
／ａｄで加圧成形し、夫々の水素吸蔵合金電極板を作製
した。このようにして得られた１４［ｊ類の水素吸蔵合
金電極板の夫々を負極とし、これに放電容量が１０００
１ＡＨの公知の焼結式ニッケル電極板を正極として組み
合わせ、アルカリ電解液として水酸化カリウム水溶液を
用いて１４種類の密閉型セルＮｏ、１〜Ｎｏ、１４を作
製した。Commercially available Ml (for example, la: 30% by weight, Ce: 45% by weight, Nd: 15% by weight, Pr: 5:li%, etc.)Ni
, C0lMn, A1 and W were selected, weighed and blended at the respective compositional components and composition ratios listed in Table 1 below,
Next, they were heated and melted in an argon arc melting furnace to obtain 14 types of alloys. Each of these alloys is mechanically crushed to a size of 32 μm or less, and 1 of various compositions having respective compositional components and atomic ratios are obtained.
Four types of hydrogen storage alloy powders were obtained. For each of these 14 types of alloy powder, 20% by weight of N1 powder as a conductive material and 5% by weight of fluororesin powder as a binder were added, mixed to form fluororesin fibers, and then crushed. Each mixture was layered to a uniform thickness on a nickel wire mesh, and
/ad to produce each hydrogen storage alloy electrode plate. Each of the 14[j class hydrogen storage alloy electrode plates obtained in this way was used as a negative electrode, and a discharge capacity of 1000
A known sintered nickel electrode plate of 1AH was combined as a positive electrode, and 14 types of closed cells No. 1 to No. 14 were prepared using an aqueous potassium hydroxide solution as an alkaline electrolyte.
これらのセルＮＧＩ〜に１４につき、０．２０の電流で
６時間充電した後、０．５０の電流でセル電圧が１．Ｏ
ｖになるまで放電するという条件で充放電サイクル試験
を行い、初期容量の６０％までの低下で寿命とするサイ
クル寿命を調べた。セル恥１〜Ｎｏ、１４の各セルの初
期の放電容量（ｎ４０７ｇ）とサイクル寿命（回）を下
記第１表に示す。After charging these cells NGI ~ 14 for 6 hours at a current of 0.20, the cell voltage rose to 1.1 at a current of 0.50. O
A charge/discharge cycle test was conducted under the condition that the battery was discharged to v, and the cycle life was determined to be the life when the battery decreased to 60% of the initial capacity. The initial discharge capacity (n407 g) and cycle life (times) of each cell with cell numbers 1 to 14 are shown in Table 1 below.
第１表
これから明らかなように、セルね８〜Ｎｏ、１２のサイ
クル寿命は３５０回以上であったに対し、従来のｔａ旧
系の合金組成をもつ水素合金電極を使用したセル馳１及
びに３は、そのサイクル寿命（回数）は僅か２０回、３
０回、８０回と著しく短い。As is clear from Table 1, the cycle life of cells No. 8 to No. 12 was more than 350 cycles, whereas the cycle life of cells No. 1 and No. 3, its cycle life (number of times) is only 20 times, 3
0 and 80 times, which is extremely short.
又、比較用のミツシェル系合金組成をもつ電極を用いた
セルＮＱ４、ぬ５、馳６．Ｎ１１７、馳１３及び馳１４
の夫々のサイクル寿命は、４５〜２００回の範囲にと７
まり、本発明の電極を用いたセルね８〜Ｎａ１２の３５
０回以上よりは著しく短いことが分かる。In addition, for comparison, cells NQ4, Nu5, Hase6. N117, Hase 13 and Hase 14
The cycle life of each ranges from 45 to 200 cycles and 7
In other words, cells No. 8 to No. 35 of Na12 using the electrodes of the present invention
It can be seen that this is significantly shorter than 0 or more times.
即ち、ＨＩＳ−Ｎｉ−Ｃｏ−Ｈｎ−ＡＩ−Ｗの６成分の
うち、少なくともＡ１かＷのいずれか１つを欠いた２〜
５戒分から成るＨｎ系水素吸蔵合金電極を用いたセルＮ
Ｑ４、社５、ＮＱ６及びぬ７のサイクル寿命は、２００
回が最大であり、又、前記６成分から成るＨｎ系水素吸
蔵合金電極を用いても、その組成式Ｈ１ｇＮｌａ Ｃｏ
ｔ Ｈｎ＊＾１４Ｗ、において、そのｄの値が対照セル
ＮＱ１３のように１．０と大きく、又、対照セル馳１４
のようにそのｅの値が０．５と大きい場合は、サイクル
寿命が２００回と低下することが認められた。多くの実
験、研究の結果、セルＮＯ，８乃至Ｎ０１２が示すよう
に、ｄの値は０，６以下であり且つｅの値は０．３以下
の組み合せにより、サイクル寿命が３５０回以上と相乗
効果が得られることが判った。即ち、Ａ１のｄの値は、
０＜ｄ≦０．６であり且つＷのｅの値はＯ＜ｅ≦０．３
であることによりサイクル寿命の延長に著しい効果があ
ることが判った。That is, 2 to 2 lacking at least one of A1 or W among the six components of HIS-Ni-Co-Hn-AI-W.
Cell N using Hn-based hydrogen storage alloy electrode consisting of five commandments
The cycle life of Q4, Sha5, NQ6 and Nu7 is 200
Moreover, even if an Hn-based hydrogen storage alloy electrode consisting of the above six components is used, its composition formula H1gNlaCo
t Hn*^14W, the value of d is as large as 1.0 like the control cell NQ13, and the value of d is as large as 1.0 like the control cell
It was found that when the value of e is as large as 0.5, the cycle life is reduced to 200 cycles. As a result of many experiments and studies, as shown in cells No. 8 to No. 012, the combination of d value of 0.6 or less and e value of 0.3 or less results in a synergistic cycle life of 350 times or more. It turned out to be effective. That is, the value of d of A1 is
0<d≦0.6 and the value of e of W is O<e≦0.3
It has been found that this has a significant effect on extending cycle life.
更に、肘に代えて８１又はＣｒを使用して、Ｗに代えて
Ｇｅを使用して試験した所、前記のＯ＜ｄ≦０．６．０
＜ｅ≦０．３の範囲で、Ａ１又はＷと同様の効果をもた
らすことが判った。Furthermore, when testing was performed using 81 or Cr instead of the elbow and Ge instead of W, the above O<d≦0.6.0 was obtained.
It was found that in the range <e≦0.3, the same effect as A1 or W is brought about.
従って、本発明においてＡｌ、Ｓｉ、Ｃｒを総括した群
をＡで表示し、ＷとＧｅｔ！−総括した群をＢで表示す
ると、本発明の水素吸蔵合金から成る電極として特に、
サイクル寿命の著しい向上を得る水素吸蔵合金は、−数
式１４１１Ｎｌ−Ｃｏｂ ｆ４ｎ、 ＡａＢ、の−数式
で表され、この場合、そのＡはＡ１、Ｓｉ及びＣｒから
成る群から撰ばれた少なくとも一種であり、ＢはＷ及び
Ｇｅから成る群から撰ばれた少なくとも一種であり、ｄ
の値はＯｄｄ≦０゜６、ｅの値はＯ＜ ｅ≦０，３の範
囲であると特定される。更に、本発明の上記組成の水素
吸蔵合金につき検討してみた所、前記の一般式ＨｉＮ
ｉ。Therefore, in the present invention, the group consisting of Al, Si, and Cr is indicated by A, and W and Get! - When the general group is denoted by B, especially as an electrode made of the hydrogen storage alloy of the present invention,
A hydrogen storage alloy that achieves a significant improvement in cycle life is represented by the formula - 1411Nl-Cob f4n, AaB, where A is at least one selected from the group consisting of A1, Si and Cr. , B is at least one selected from the group consisting of W and Ge, and d
The value of is specified as Odd≦0°6, and the value of e is specified as being in the range of O<e≦0,3. Further, after studying the hydrogen storage alloy of the present invention having the above composition, we found that the general formula HiN
i.
Ｃｏｂ １４ｎｃＡａ Ｂ、で示される合金は、ＣａＣ
ＩＪ ｓ型の六方晶ｍ遣を持ち、この六方晶構造を持つ
合金では化学量論的にＣＤ５ （但し、Ｃは上記組成
式でＨｎを、又、ＤはＮｉ−Ｃｏ−Ｈｎ−＾−Ｂ合金を
表す）から若干ずれた組成でも六方晶構造を維持するが
、Ｄの組成比が±１０％より大きくずれるとこの構造を
保てず、水素吸蔵合金としての特性が損なわれることが
分かった。よって、上記組成式において、４．５≦ａ＋
ｂ＋ｃ＋ｄ＋ｅ≦５，５の範囲とする必要がある。The alloy designated Cob 14ncAa B, is CaC
IJ has a hexagonal crystal structure of the s type, and the alloy with this hexagonal crystal structure has a stoichiometric CD5 (however, C is Hn in the above composition formula, and D is Ni-Co-Hn-^-B Although the hexagonal crystal structure is maintained even if the composition slightly deviates from the D composition (representing the alloy), it was found that if the composition ratio of D deviates by more than ±10%, this structure cannot be maintained and the properties as a hydrogen storage alloy are impaired. . Therefore, in the above compositional formula, 4.5≦a+
It is necessary to set the range of b+c+d+e≦5.5.
このように本発明によるときは、ＨＩｊＮｌａ ＣＯｉ
＝ＭｎｅＣ０１＝なる一般組成式（償し、Ｈ旧よミツシ
ュメタル、ＡはＡ１、Ｓｉ及びＣｒから成る群より撰ば
れた少なくとも１種、ＢはＷ及びＧｅから成る群より撰
ばれた少なくとも１種、且つ４．５≦ａ＋ｂ＋ｃ＋ｄ＋
ｅ≦５．５．０＜ｄ≦０．６．０＜ｅ≦０゜３）で表さ
れる合金を、アルカリ蓄電池の負極として用いるときは
、従来のＬａＮ ｉ、ＬａＮｌ２ＣＯ３、ＬａＮ１＜、
ｓ Ｈｎｏ、ｑなどに比し電池のサイクル寿命を著しく
向上し得る効果を有する。Thus, according to the present invention, HIjNla COi
=MneC01= General compositional formula (Atone, H old Mitsushmetal, A is at least one selected from the group consisting of A1, Si and Cr, B is at least one selected from the group consisting of W and Ge, and 4.5≦a+b+c+d+
When using an alloy represented by e≦5.5.0<d≦0.6.0<e≦0゜3) as a negative electrode of an alkaline storage battery, conventional LaN i, LaNl2CO3, LaN1<,
It has the effect of significantly improving the cycle life of the battery compared to Hno, q, etc.
Claims (1)
（但し、Ｍｍはミッシュメタル、ＡはＡｌ、Ｓｉ及びＣ
ｒから成る群より撰択された少なくとも１種、ＢはＷ及
びＧｅから成る群より撰択された少なくとも１種、且つ
４．５≦ａ＋ｂ＋ｃ＋ｄ＋ｅ≦５．５、０＜ｄ≦０．６
、０＜ｅ≦０．３）で表される水素吸蔵合金から成るこ
とを特徴とするアルカリ蓄電池用水素吸蔵電極。1. General formula MmNi_aCO_bMn_cA_dB_e
(However, Mm is misch metal, A is Al, Si and C.
At least one type selected from the group consisting of r, B is at least one type selected from the group consisting of W and Ge, and 4.5≦a+b+c+d+e≦5.5, 0<d≦0.6
, 0<e≦0.3).
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1264238A JPH03126832A (en) | 1989-10-11 | 1989-10-11 | Hydrogen occluding electrode for alkaline storage battery |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP1264238A JPH03126832A (en) | 1989-10-11 | 1989-10-11 | Hydrogen occluding electrode for alkaline storage battery |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH03126832A true JPH03126832A (en) | 1991-05-30 |
| JPH0567694B2 JPH0567694B2 (en) | 1993-09-27 |
Family
ID=17400406
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP1264238A Granted JPH03126832A (en) | 1989-10-11 | 1989-10-11 | Hydrogen occluding electrode for alkaline storage battery |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH03126832A (en) |
Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH01162741A (en) * | 1987-12-18 | 1989-06-27 | Sanyo Electric Co Ltd | Hydrogen occluding alloy electrode |
| JPH0268856A (en) * | 1988-09-01 | 1990-03-08 | Sanyo Electric Co Ltd | Hydrogen occluded alloy electrode |
| JPH02220356A (en) * | 1989-02-21 | 1990-09-03 | Sanyo Electric Co Ltd | Hydrogen storage alloy electrode for alkaline battery and manufacture thereof |
| JPH02277737A (en) * | 1989-04-18 | 1990-11-14 | Sanyo Electric Co Ltd | Electrode made of hydrogen storage alloy |
-
1989
- 1989-10-11 JP JP1264238A patent/JPH03126832A/en active Granted
Patent Citations (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH01162741A (en) * | 1987-12-18 | 1989-06-27 | Sanyo Electric Co Ltd | Hydrogen occluding alloy electrode |
| JPH0268856A (en) * | 1988-09-01 | 1990-03-08 | Sanyo Electric Co Ltd | Hydrogen occluded alloy electrode |
| JPH02220356A (en) * | 1989-02-21 | 1990-09-03 | Sanyo Electric Co Ltd | Hydrogen storage alloy electrode for alkaline battery and manufacture thereof |
| JPH02277737A (en) * | 1989-04-18 | 1990-11-14 | Sanyo Electric Co Ltd | Electrode made of hydrogen storage alloy |
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0567694B2 (en) | 1993-09-27 |
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