JP3443270B2 - Hydrogen storage alloy - Google Patents
Hydrogen storage alloyInfo
- Publication number
- JP3443270B2 JP3443270B2 JP04831397A JP4831397A JP3443270B2 JP 3443270 B2 JP3443270 B2 JP 3443270B2 JP 04831397 A JP04831397 A JP 04831397A JP 4831397 A JP4831397 A JP 4831397A JP 3443270 B2 JP3443270 B2 JP 3443270B2
- Authority
- JP
- Japan
- Prior art keywords
- hydrogen storage
- storage alloy
- alloy
- hydrogen
- general formula
- 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 - Fee Related
Links
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims description 51
- 239000001257 hydrogen Substances 0.000 title claims description 50
- 229910052739 hydrogen Inorganic materials 0.000 title claims description 50
- 229910045601 alloy Inorganic materials 0.000 title claims description 48
- 239000000956 alloy Substances 0.000 title claims description 48
- 229910052748 manganese Inorganic materials 0.000 claims description 6
- 229910052804 chromium Inorganic materials 0.000 claims description 5
- 229910052802 copper Inorganic materials 0.000 claims description 5
- 229910052742 iron Inorganic materials 0.000 claims description 5
- 229910001068 laves phase Inorganic materials 0.000 claims description 5
- 238000010791 quenching Methods 0.000 claims description 5
- 230000000171 quenching effect Effects 0.000 claims description 5
- 229910052720 vanadium Inorganic materials 0.000 claims description 5
- 229910052725 zinc Inorganic materials 0.000 claims description 5
- 229910052761 rare earth metal Inorganic materials 0.000 claims description 4
- 239000000155 melt Substances 0.000 claims 1
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 12
- 238000010521 absorption reaction Methods 0.000 description 8
- 229910052759 nickel Inorganic materials 0.000 description 7
- 239000000203 mixture Substances 0.000 description 6
- 230000004913 activation Effects 0.000 description 5
- 229910010380 TiNi Inorganic materials 0.000 description 3
- 238000003795 desorption Methods 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 229910002056 binary alloy Inorganic materials 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 229910052751 metal Inorganic materials 0.000 description 2
- 239000002184 metal Substances 0.000 description 2
- 238000000034 method Methods 0.000 description 2
- 238000001556 precipitation Methods 0.000 description 2
- 229920006395 saturated elastomer Polymers 0.000 description 2
- 238000006467 substitution reaction Methods 0.000 description 2
- 229910052684 Cerium Inorganic materials 0.000 description 1
- 229910052692 Dysprosium Inorganic materials 0.000 description 1
- 229910052691 Erbium Inorganic materials 0.000 description 1
- 229910052693 Europium Inorganic materials 0.000 description 1
- 229910052688 Gadolinium Inorganic materials 0.000 description 1
- 229910052689 Holmium Inorganic materials 0.000 description 1
- 229910001122 Mischmetal Inorganic materials 0.000 description 1
- 229910052779 Neodymium Inorganic materials 0.000 description 1
- 229910003310 Ni-Al Inorganic materials 0.000 description 1
- 229910052777 Praseodymium Inorganic materials 0.000 description 1
- 229910052772 Samarium Inorganic materials 0.000 description 1
- 229910052771 Terbium Inorganic materials 0.000 description 1
- 229910052775 Thulium Inorganic materials 0.000 description 1
- 229910052769 Ytterbium Inorganic materials 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 150000002431 hydrogen Chemical class 0.000 description 1
- 229910052746 lanthanum Inorganic materials 0.000 description 1
- DOARWPHSJVUWFT-UHFFFAOYSA-N lanthanum nickel Chemical compound [Ni].[La] DOARWPHSJVUWFT-UHFFFAOYSA-N 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 239000007773 negative electrode material Substances 0.000 description 1
Landscapes
- Battery Electrode And Active Subsutance (AREA)
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、水素貯蔵システ
ム、ヒートポンプ、アクチュエータ、ニッケル水素電池
等に用いられる水素吸蔵合金に関し、特に、良好な水素
吸放出特性を有する新規な水素貯蔵合金に関するもので
ある。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a hydrogen storage alloy used in hydrogen storage systems, heat pumps, actuators, nickel hydrogen batteries, etc., and more particularly to a novel hydrogen storage alloy having good hydrogen storage / release characteristics. .
【０００２】[0002]
【従来の技術】従来より、水素吸蔵合金として、ランタ
ン・ニッケル(ＬａＮｉ5)系合金等の２元合金や、これ
を多成分化した擬２元合金が知られており、例えば水素
吸蔵システム等に広く応用されている。又、希土類元素
(Ｌａ、Ｃｅ、Ｐｒ、Ｎｄ、Ｐｍ、Ｓｍ、Ｅｕ、Ｇｄ、
Ｔｂ、Ｄｙ、Ｈｏ、Ｅｒ、Ｔｍ、Ｙｂ、Ｌｎ)の複数種
の混合物であるミッシュメタル(Ｍｍ)と、Ｎｉ、Ｍｎ、
Ａｌ等の金属元素とからなるＡＢ5型水素吸蔵合金が開
発され、例えばニッケル水素電池の負極材料として用い
られている。2. Description of the Related Art Conventionally, as hydrogen storage alloys, binary alloys such as lanthanum-nickel (LaNi 5 ) alloys and pseudo-binary alloys having multiple components have been known. For example, hydrogen storage systems. Widely applied to. Also, rare earth elements
(La, Ce, Pr, Nd, Pm, Sm, Eu, Gd,
Tb, Dy, Ho, Er, Tm, Yb, Ln) is a mixture of a plurality of types of misch metal (Mm), Ni, Mn,
An AB 5 type hydrogen storage alloy composed of a metal element such as Al has been developed and used, for example, as a negative electrode material of a nickel hydrogen battery.
【０００３】ところで、水素吸蔵合金を水素貯蔵システ
ム等に応用する場合、水素吸蔵合金の重量やコストが問
題となり、これらの点で、従来より知られている水素吸
蔵合金は充分に満足し得るものとは言えなかった。By the way, when the hydrogen storage alloy is applied to a hydrogen storage system or the like, the weight and cost of the hydrogen storage alloy pose a problem. From these points, the conventionally known hydrogen storage alloy is sufficiently satisfactory. I couldn't say that.
【０００４】これに対し、一般式Ｔｉ3ＮｉxＡｌ
1-x(０.００５≦ｘ≦０.３)、或いはＴｉ3 -xＮｉxＡｌ
(０.００５≦ｘ≦０.３)で表わされる水素吸蔵合金が知
られている(特開平５６−１６６３５５号)。該水素吸蔵
合金は、その構成元素として、比較的軽量であって、且
つ安価に入手出来るＴｉ、Ａｌ及びＮｉを用いており、
重量及びコストの点で優れている。On the other hand, the general formula Ti 3 Ni x Al
1-x (0.005 ≤ x ≤ 0.3) or Ti 3 -x Ni x Al
A hydrogen storage alloy represented by (0.005 ≦ x ≦ 0.3) is known (Japanese Patent Laid-Open No. 56-166355). The hydrogen storage alloy uses, as its constituent elements, Ti, Al and Ni, which are relatively lightweight and can be obtained at low cost,
Excellent in weight and cost.
【０００５】[0005]
【発明が解決しようとする課題】しかしながら、上記一
般式で表わされる従来の水素吸蔵合金においては、水素
吸放出特性の点で充分に満足しうるものとは言えなかっ
た。本発明の目的は、Ｔｉ−Ｎｉ−Ａｌ系合金におい
て、充分な水素吸放出特性が得られる合金組成を明らか
にすることである。However, the conventional hydrogen storage alloy represented by the above general formula cannot be said to be sufficiently satisfactory in terms of hydrogen absorption / desorption characteristics. An object of the present invention is to clarify the alloy composition of Ti-Ni-Al based alloys that can obtain sufficient hydrogen absorption / desorption characteristics.
【０００６】[0006]
【課題を解決する為の手段】本発明に係る第１の水素吸
蔵合金は、一般式ＴｉＮｉxＡｌy(ｘ＝０.８〜１.２、
ｙ＝０.７〜１.２)で表わされ、Ｃ１４型ラーベス相構
造を有するものである。これまでに、一般式ＴｉＮｉx
Ａｌy(ｘ＝０.８〜１.２、ｙ＝０.７〜１.２)で表わさ
れる合金の水素吸放出能力は確認されていなかったが、
本発明者らが鋭意研究を重ねた結果、該合金の水素吸放
出能力を初めて定量的に確認したものである。The first hydrogen storage alloy according to the present invention has a general formula of TiNi x Al y (x = 0.8 to 1.2,
y = 0.7 to 1.2) and has a C14 type Laves phase structure. So far, the general formula TiNi x
Al y (x = 0.8~1.2, y = 0.7~1.2) is absorbing and releasing capacity of hydrogen of the alloy represented by has not been confirmed,
As a result of intensive studies by the present inventors, the present inventors quantitatively confirmed the hydrogen absorbing / releasing ability of the alloy for the first time.
【０００７】又、本発明に係る第２の水素吸蔵合金は、
一般式Ｔｉ(ＮｉxＡｌy)1-zＭz(０.８≦ｘ≦１.２、０.
７≦ｙ≦１.２、０＜ｚ≦０.２、ＭはＶ、Ｃｒ、Ｍｎ、
Ｆｅ、Ｃｏ、Ｃｕ、Ｚｎ及び希土類元素からなる群から
選ばれた少なくとも一種の元素)で表わされ、Ｃ１４型
ラーベス相構造を有するものである。該水素吸蔵合金
は、上記第１の水素吸蔵合金のＮｉ若しくはＡｌの一部
をＶ、Ｃｒ、Ｍｎ、Ｆｅ、Ｃｏ、Ｃｕ、Ｚｎ及び希土類
元素からなる群から選ばれた少なくとも一種の元素で置
換したものである。これによって、母相中に第２相が析
出し、該析出相によって水素吸蔵合金の活性化が促進さ
れる。The second hydrogen storage alloy according to the present invention is
The general formula Ti (NixAly) 1-zMz ( 0.8≤x≤1.2, 0.0.
7 ≦ y ≦ 1.2, 0 <z ≦ 0.2 , M is V, Cr, Mn,
Fe, Co, Cu, Zn and at least one element selected from the group consisting of rare earth elements) and has a C14 type Laves phase structure. In the hydrogen storage alloy, a part of Ni or Al of the first hydrogen storage alloy is replaced with at least one element selected from the group consisting of V, Cr, Mn, Fe, Co, Cu, Zn and rare earth elements. It was done. As a result, the second phase is precipitated in the mother phase, and the precipitation phase promotes activation of the hydrogen storage alloy.
【０００８】尚、上記第１或いは第２の水素吸蔵合金の
溶湯を１００℃／秒以上の速度で急冷することによっ
て、合金組織が均質化され、サイクル寿命が向上する。By quenching the molten metal of the first or second hydrogen storage alloy at a rate of 100 ° C./sec or more, the alloy structure is homogenized and the cycle life is improved.
【０００９】[0009]
【発明の効果】本発明に係る水素吸蔵合金は、重量及び
コストの点のみならず、水素吸放出特性の点においても
優れている。The hydrogen storage alloy according to the present invention is excellent not only in weight and cost, but also in hydrogen storage / release characteristics.
【００１０】[0010]
【発明の実施の形態】第１実施例
組成がＴｉＮｉxＡｌy(ｘ＝０.６〜１.４、ｙ＝０.６〜
１.４)となる様に、Ｔｉ、Ｎｉ、及びＡｌの粉末を秤量
混合し、これによって得られる組成比の異なる各混合物
をアーク溶解法によって溶融せしめた後、真空雰囲気下
で、１０５０℃、８時間の熱処理を施した。これによっ
て得られた各合金塊を粉砕して、合金粉末を作製し、各
合金粉末を反応容器に夫々充填して、１５０℃で３時間
の真空排気を行なった。その後、各反応容器に４０ａｔ
ｍの水素ガスを導入し、初期活性化を行ない、その際の
水素吸収量を夫々測定した。その結果を下記表１に示
す。BEST MODE FOR CARRYING OUT THE INVENTION First Embodiment The composition is TiNi x Al y (x = 0.6 to 1.4, y = 0.6 to
1.4), Ti, Ni, and Al powders were weighed and mixed, and the respective mixtures with different composition ratios thus obtained were melted by an arc melting method, and then, at 1050 ° C. in a vacuum atmosphere, Heat treatment was performed for 8 hours. The alloy lumps thus obtained were crushed to prepare alloy powders, the alloy powders were filled in the respective reaction vessels, and vacuum evacuation was performed at 150 ° C. for 3 hours. After that, 40at in each reaction vessel
m hydrogen gas was introduced, initial activation was performed, and the amount of hydrogen absorbed at that time was measured. The results are shown in Table 1 below.
【００１１】[0011]
【表１】 [Table 1]
【００１２】表１から明らかな様に、ｘが０.８〜１.２
の範囲であって、且つｙが０.７〜１.２の範囲におい
て、他の範囲よりも水素吸収量が著しく増大している。
これは、他の範囲では、水素吸収能力を有しない副相が
増加し、完全なＣ１４型ラーベス相構造が得られないた
めと考えられる。As is clear from Table 1, x is 0.8 to 1.2.
In the above range and y is in the range of 0.7 to 1.2, the hydrogen absorption amount is remarkably increased as compared with the other ranges.
This is considered to be because, in other ranges, the number of sub-phases having no hydrogen absorption capacity increased, and a complete C14-type Laves phase structure could not be obtained.
【００１３】又、表１から明らなか様に、ｘが０.９〜
１.１の範囲であって、且つｙが０.８〜１.２の範囲に
おいて、０.４(Ｈ／Ｍ)を越える高い水素吸収量が得ら
れている。更に、ｘが０.９〜１.１の範囲であって、且
つｙが１.０〜１.１の範囲において、０.８(Ｈ／Ｍ)を
越える極めて高い水素吸収量が得られており、これらの
範囲が望ましいことがわかる。As is clear from Table 1, x is 0.9 to
In the range of 1.1 and y of 0.8 to 1.2, a high hydrogen absorption amount exceeding 0.4 (H / M) was obtained. Furthermore, when x is in the range of 0.9 to 1.1 and y is in the range of 1.0 to 1.1, an extremely high hydrogen absorption amount exceeding 0.8 (H / M) is obtained. Therefore, it is understood that these ranges are desirable.
【００１４】第２実施例
組成がＴｉ(Ｎｉ1.0Ａｌ1.0)0.9Ｍ0.1(ＭはＶ、Ｃｒ、
Ｍｎ、Ｆｅ、Ｃｏ、Ｃｕ、Ｚｎ、又はＲＥ)で表わされ
る水素吸蔵合金を、第１実施例と同様の条件で作製し、
第１実施例と同様の条件で、初期活性化特性を測定し
た。又、第１実施例の水素吸蔵合金についても、同様に
初期活性化特性を測定した。これらの結果を下記表２に
示す。又、表２をグラフ化して図１に示す。 Second Embodiment The composition is Ti (Ni 1.0 Al 1.0 ) 0.9 M 0.1 (M is V, Cr,
A hydrogen storage alloy represented by Mn, Fe, Co, Cu, Zn, or RE) was prepared under the same conditions as in the first embodiment,
The initial activation characteristics were measured under the same conditions as in the first example. The initial activation characteristics of the hydrogen storage alloy of Example 1 were also measured in the same manner. The results are shown in Table 2 below. Further, Table 2 is shown as a graph in FIG.
【００１５】[0015]
【表２】 [Table 2]
【００１６】表２及び図１から明らかな様に、Ｎｉ若し
くはＡｌの一部をＶ、Ｃｒ、Ｍｎ、Ｆｅ、Ｃｏ、Ｃｕ、
Ｚｎ、又はＲＥで置換した水素吸蔵合金においては、何
れも約３時間で水素吸収量が飽和状態に達しているのに
対し、元素置換のない水素吸蔵合金においては、４時間
が経過しても飽和状態に達していない。これは、元素置
換によって、水素吸蔵合金の母相中に第２相が析出し、
該析出相によって水素吸蔵合金の活性化が促進されるか
らである。As is clear from Table 2 and FIG. 1, a part of Ni or Al is V, Cr, Mn, Fe, Co, Cu,
In each of the hydrogen storage alloys substituted with Zn or RE, the hydrogen absorption amount reached the saturated state in about 3 hours, whereas in the hydrogen storage alloys without element substitution, even after 4 hours had elapsed. Not saturated. This is because the second phase is precipitated in the mother phase of the hydrogen storage alloy by element replacement,
This is because the precipitation phase promotes activation of the hydrogen storage alloy.
【００１７】第３実施例
ＴｉＮｉＡｌ合金を、第１実施例と同様の条件で２サン
プル作製し、一方のサンプルには、ロール急冷法によっ
て、約１０００℃／ｍｉｎの急冷を施した(急冷合金)。
尚、他方のサンプルの冷却速度は通常の約３０℃／ｍｉ
ｎである(通常合金)。そして、急冷合金と通常合金の夫
々についてサイクル特性の測定を行なった。測定におい
ては、先ずサンプルの温度を０℃に保持して３０分間の
真空排気の後、１５ａｔｍの水素ガスを３０分間印加し
て、水素を吸収させる処理を１サイクルとした。これら
の結果を下記表３に示す。又、表３をグラフ化して図２
に示す。 Third Embodiment Two samples of TiNiAl alloy were prepared under the same conditions as in the first embodiment, and one sample was rapidly cooled at about 1000 ° C./min by a roll quenching method (quenched alloy). .
The cooling rate of the other sample was about 30 ° C / mi, which is the normal rate.
n (normal alloy). Then, the cycle characteristics of the quenched alloy and the normal alloy were measured. In the measurement, first, the temperature of the sample was kept at 0 ° C., vacuum exhaustion was performed for 30 minutes, and then 15 atm of hydrogen gas was applied for 30 minutes to absorb hydrogen, which was one cycle. The results are shown in Table 3 below. Also, Table 3 is graphed and shown in FIG.
Shown in.
【００１８】[0018]
【表３】 [Table 3]
【００１９】表３及び図２から明らかなように、急冷合
金は、通常合金に比べて水素吸収量の低下が緩やかとな
っており、サイクル特性が向上している。これは、水素
吸蔵合金を溶湯の状態から急冷することによって、組織
が均質化され、水素吸放出時に発生する合金格子の歪み
が緩和されるためと考えられる。As is clear from Table 3 and FIG. 2, the quenched alloy has a more gradual decrease in the amount of hydrogen absorbed than the normal alloy, and the cycle characteristics are improved. This is considered to be because the structure is homogenized by quenching the hydrogen storage alloy from the molten state and the strain of the alloy lattice generated at the time of hydrogen absorption and desorption is relaxed.
【００２０】上記実施の形態の説明は、本発明を説明す
るためのものであって、特許請求の範囲に記載の発明を
限定し、或は範囲を減縮する様に解すべきではない。
又、本発明の各部構成は上記実施の形態に限らず、特許
請求の範囲に記載の技術的範囲内で種々の変形が可能で
あることは勿論である。The above description of the embodiments is for explaining the present invention, and should not be construed as limiting the invention described in the claims or reducing the scope.
Further, it goes without saying that the configuration of each part of the present invention is not limited to the above-described embodiment, and various modifications can be made within the technical scope described in the claims.
【図１】本発明に係る水素吸蔵合金の元素置換による効
果を表わすグラフである。FIG. 1 is a graph showing an effect of element substitution of a hydrogen storage alloy according to the present invention.
【図２】本発明に係る水素吸蔵合金の急冷による効果を
表わすグラフである。FIG. 2 is a graph showing the effect of quenching the hydrogen storage alloy according to the present invention.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 米津 育郎 大阪府守口市京阪本通２丁目５番５号 三洋電機株式会社内 (72)発明者 西尾 晃治 大阪府守口市京阪本通２丁目５番５号 三洋電機株式会社内 (56)参考文献 特開 平７−90464（ＪＰ，Ａ) 特開 平７−235304（ＪＰ，Ａ) 特開 平８−104940（ＪＰ，Ａ) 特開 平９−49039（ＪＰ，Ａ) (58)調査した分野(Int.Cl.7，ＤＢ名) C22C 1/00 - 49/14 ─────────────────────────────────────────────────── ─── Continuation of the front page (72) Inventor Ichiro Yonezu 2-5-5 Keihan Hondori, Moriguchi City, Osaka Prefecture Sanyo Electric Co., Ltd. (72) Inventor Koji Nishio 2-5 Keihan Hondori, Moriguchi City, Osaka Prefecture No. 5 within Sanyo Electric Co., Ltd. (56) Reference JP-A-7-90464 (JP, A) JP-A-7-235304 (JP, A) JP-A-8-104940 (JP, A) JP-A-9- 49039 (JP, A) (58) Fields surveyed (Int.Cl. 7 , DB name) C22C 1/00-49/14
Claims (3)
２、ｙ＝０.７〜１.２)で表わされ、Ｃ１４型ラーベス
相構造を有する水素吸蔵合金。1. The general formula TiNixAly (x = 0.8-1.
2, y = 0.7 to 1.2), and a hydrogen storage alloy having a C14 type Laves phase structure.
ｘ≦１.２、０.７≦ｙ≦１.２、０＜ｚ≦０.２、Ｍは
Ｖ、Ｃｒ、Ｍｎ、Ｆｅ、Ｃｏ、Ｃｕ、Ｚｎ及び希土類元
素からなる群から選ばれた少なくとも一種の元素)で表
わされ、Ｃ１４型ラーベス相構造を有する水素吸蔵合
金。 2. The general formula Ti (NixAly) 1-zMz ( 0.8 ≦
x ≦ 1.2, 0.7 ≦ y ≦ 1.2, 0 <z ≦ 0.2 , M is at least selected from the group consisting of V, Cr, Mn, Fe, Co, Cu, Zn and rare earth elements. A hydrogen storage alloy having a C14 type Laves phase structure.
の溶湯を１００℃／秒以上の速度で急冷してなる水素吸
蔵合金。3. A hydrogen storage alloy obtained by quenching the melt of the alloy according to claim 1 or 2 at a rate of 100 ° C./sec or more.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP04831397A JP3443270B2 (en) | 1997-03-03 | 1997-03-03 | Hydrogen storage alloy |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP04831397A JP3443270B2 (en) | 1997-03-03 | 1997-03-03 | Hydrogen storage alloy |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH10245648A JPH10245648A (en) | 1998-09-14 |
| JP3443270B2 true JP3443270B2 (en) | 2003-09-02 |
Family
ID=12799936
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP04831397A Expired - Fee Related JP3443270B2 (en) | 1997-03-03 | 1997-03-03 | Hydrogen storage alloy |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3443270B2 (en) |
-
1997
- 1997-03-03 JP JP04831397A patent/JP3443270B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPH10245648A (en) | 1998-09-14 |
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