JP2794477B2 - Hydrogen storage alloy - Google Patents
Hydrogen storage alloyInfo
- Publication number
- JP2794477B2 JP2794477B2 JP2107458A JP10745890A JP2794477B2 JP 2794477 B2 JP2794477 B2 JP 2794477B2 JP 2107458 A JP2107458 A JP 2107458A JP 10745890 A JP10745890 A JP 10745890A JP 2794477 B2 JP2794477 B2 JP 2794477B2
- Authority
- JP
- Japan
- Prior art keywords
- hydrogen storage
- hydrogen
- storage alloy
- alloy
- pressure
- 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
- 239000001257 hydrogen Substances 0.000 title claims description 55
- 229910052739 hydrogen Inorganic materials 0.000 title claims description 55
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims description 54
- 239000000956 alloy Substances 0.000 title claims description 47
- 229910045601 alloy Inorganic materials 0.000 title claims description 43
- PXHVJJICTQNCMI-UHFFFAOYSA-N nickel Substances [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 12
- 239000000203 mixture Substances 0.000 description 10
- 238000005057 refrigeration Methods 0.000 description 10
- 230000000052 comparative effect Effects 0.000 description 9
- 238000010521 absorption reaction Methods 0.000 description 6
- 229910052761 rare earth metal Inorganic materials 0.000 description 5
- 238000006467 substitution reaction Methods 0.000 description 5
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 4
- 229910052772 Samarium Inorganic materials 0.000 description 4
- 238000005516 engineering process Methods 0.000 description 4
- 238000006243 chemical reaction Methods 0.000 description 3
- 238000003795 desorption Methods 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 229910052746 lanthanum Inorganic materials 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- KZUNJOHGWZRPMI-UHFFFAOYSA-N samarium atom Chemical compound [Sm] KZUNJOHGWZRPMI-UHFFFAOYSA-N 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- 229910052786 argon Inorganic materials 0.000 description 2
- 238000005984 hydrogenation reaction Methods 0.000 description 2
- 238000002844 melting Methods 0.000 description 2
- 230000008018 melting Effects 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- 229910052779 Neodymium Inorganic materials 0.000 description 1
- 229910000990 Ni alloy Inorganic materials 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 239000000498 cooling water Substances 0.000 description 1
- 230000002542 deteriorative effect Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- FZLIPJUXYLNCLC-UHFFFAOYSA-N lanthanum atom Chemical compound [La] FZLIPJUXYLNCLC-UHFFFAOYSA-N 0.000 description 1
- DOARWPHSJVUWFT-UHFFFAOYSA-N lanthanum nickel Chemical compound [Ni].[La] DOARWPHSJVUWFT-UHFFFAOYSA-N 0.000 description 1
- 239000008204 material by function Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 150000002910 rare earth metals Chemical class 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
Landscapes
- Hydrogen, Water And Hydrids (AREA)
- Battery Electrode And Active Subsutance (AREA)
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に関し、特に熱駆動型冷凍シス
テムに用いて好適なる希土類系水素吸蔵合金の改良に関
する。The present invention relates to a hydrogen storage alloy, and more particularly to an improvement in a rare earth hydrogen storage alloy suitable for use in a heat driven refrigeration system.
（ロ）従来の技術 近年、化石資源枯渇によるエネルギー事情の悪化及び
炭酸ガスによる地球温暖化現象の顕在化等の環境問題に
より、現在の石油、電力を中心とするエネルギーシステ
ムの代替として資源的に無尽蔵、かつクリーンな水素を
用いたエネルギーシステムが有望視され、種々の水素エ
ネルギー技術の開発が盛んに行われている。(B) Conventional technology In recent years, due to the deteriorating energy situation due to the depletion of fossil resources and the emergence of global warming phenomena due to carbon dioxide gas, resources are being replaced as alternatives to the current oil and power-based energy systems. Energy systems using inexhaustible and clean hydrogen are promising, and various hydrogen energy technologies are being actively developed.
この中で、とりわけ大量の反応熱を伴って水素を大量
に吸収・放出する水素吸蔵合金材料は、水素エネルギー
システムの要素技術である水素の貯蔵、輸送及び熱・機
械エネルギー変換用の機能材料として極めて重要であ
る。Among them, hydrogen storage alloy materials, which absorb and release large amounts of hydrogen with a large amount of heat of reaction, are used as functional materials for hydrogen storage, transport, and thermal / mechanical energy conversion, which are element technologies of hydrogen energy systems. Very important.
ところで、上記の水素吸放出に伴う反応熱を利用する
熱駆動型冷凍システムに用いる水素吸蔵合金に於ては、
その平衡水素圧力は高いほうがよいが、安全上の面から
圧力約10atmが適当である。したがって、システムの構
成上必要不可欠である冷却水に用いる市水の温度が20〜
35℃であることから、平衡水素圧力は20〜35℃の範囲内
で約10atmである必要がある。また、０度以下の出熱を
得るために、HSファクター（一定量〔0.9wt％〕の水素
を可逆的に吸蔵、放出するために必要な圧力の自然対数
差）が1.0以下であることが必要である。By the way, in the hydrogen storage alloy used in the heat driven refrigeration system utilizing the reaction heat accompanying the hydrogen absorption and desorption described above,
The higher the equilibrium hydrogen pressure, the better, but a pressure of about 10 atm is appropriate for safety. Therefore, the temperature of city water used for cooling water, which is indispensable for
Since it is 35 ° C, the equilibrium hydrogen pressure needs to be about 10 atm in the range of 20 to 35 ° C. Also, in order to obtain a heat output of 0 degree or less, the HS factor (the natural logarithm of the pressure required to reversibly store and release a fixed amount [0.9 wt%] of hydrogen) may be 1.0 or less. is necessary.
上記のような要求に応ずるべく、種々開発されてきた
水素吸蔵合金の中で、平衡圧力の面から熱駆動型冷凍シ
ステムに適した合金としては、特開昭60−197835号公報
に示される希土類−Ni系合金が挙げられる。Among the hydrogen storage alloys that have been variously developed to meet the above-mentioned requirements, alloys suitable for a heat-driven refrigeration system from the viewpoint of equilibrium pressure are rare earth elements described in JP-A-60-197835. -Ni-based alloys.
（ハ）発明が解決しようとする課題 上述のように、平衡圧力の点で改良されたものは出現
しているが、熱駆動型冷凍システム用として、平衡圧
力、HSファクターの双方ともに優れた合金系は未だ開発
されていない。(C) Problems to be Solved by the Invention As described above, those improved in terms of equilibrium pressure have emerged, but alloys that are excellent in both equilibrium pressure and HS factor for heat-driven refrigeration systems. The system has not been developed yet.
本発明は、上記の点に鑑みなされたものであって、熱
駆動型冷凍システムに対して要求される比較的高い平衡
水素圧力（20〜35℃で約10atm）、優れたHSファクター
（1.0以下）を兼ね備えた水素吸蔵合金材料を提供する
ことを目的とする。The present invention has been made in view of the above points, and requires a relatively high equilibrium hydrogen pressure (about 10 atm at 20 to 35 ° C.) and an excellent HS factor (1.0 or less) required for a heat driven refrigeration system. It is an object of the present invention to provide a hydrogen storage alloy material having the above characteristics.
（ニ）課題を解決するための手段 このため、本発明の水素吸蔵合金は、組成がLa1-xSmx
Ni5で表され、希土類元素であるサマリウム（Sm）の含
有量Ｘを、0.4≦Ｘ≦0.55としたものである。(D) Means for Solving the Problems For this reason, the hydrogen storage alloy of the present invention has a composition of La 1-x Sm x
The content X of samarium (Sm), which is represented by Ni 5 and is a rare earth element, is set to 0.4 ≦ X ≦ 0.55.
（ホ）作 用 大量の水素吸収・放出と優れたHSファクターを持つ水
素吸蔵合金であるランタン−ニッケル系合金（LaNi5）
は常温で2atm程度の低い平衡圧力しか持たない。このた
め、ランタン（La）に対し、平衡水素圧力を大きく上昇
させ、HSファクターを維持し得るサマリウム（Sm）で置
換することにより、熱駆動型冷凍システムに対して要求
される比較的高い平衡水素圧力（20〜35℃で約10atm）
と優れたHSファクター（1.0以下）を兼ね備えた水素吸
蔵合金が得られる。(E) Action Lanthanum-nickel alloy (LaNi 5 ), a hydrogen storage alloy with a large amount of hydrogen absorption / desorption and an excellent HS factor
Has only a low equilibrium pressure of about 2 atm at room temperature. For this reason, by increasing the equilibrium hydrogen pressure of lanthanum (La) significantly and replacing it with samarium (Sm) that can maintain the HS factor, the relatively high equilibrium hydrogen required for the heat driven refrigeration system is obtained. Pressure (about 10atm at 20-35 ℃)
And a hydrogen storage alloy having an excellent HS factor (1.0 or less).
なお、Smによる置換量が0.4以下であると、平衡圧力
が低くなり過ぎるため実用には不適切であり、0.55以上
であると、HSファクターが1.0以上となるため、実用に
は供しなくなる。If the substitution amount with Sm is 0.4 or less, the equilibrium pressure becomes too low, which is inappropriate for practical use. If the substitution amount is 0.55 or more, the HS factor becomes 1.0 or more, so that it is not practically used.
（ヘ）実施例 実施例１ 所定量のLaと、希土類元素のサマリウム（Sm）と及び
Niの粉末混合体をプレスした後、アルゴンアーク溶解炉
にてこれを溶解し、第１表のＤ〜Ｆに示す本発明の水素
吸蔵合金に係る組成（La1-XSmXNi5）のボタン状合金鋳
塊を得た。また、ここで用いた合金材料はいずれも99.9
％の純度を持つものである。(F) Examples Example 1 A predetermined amount of La, a rare earth element samarium (Sm), and
After pressing the Ni powder mixture, it was melted in an argon arc melting furnace, and the composition (La 1-X Sm X Ni 5 ) of the hydrogen storage alloy of the present invention shown in DF of Table 1 was obtained. A button-shaped alloy ingot was obtained. The alloy materials used here were all 99.9%.
% Purity.
参考例 なお、第１表のＡ〜Ｃには、LaおよびNiに混合する希
土類元素としてイットリウム（Ｙ）を用いた場合の水素
吸蔵合金をも参考例として、挙げている。Reference Examples In Tables A to C, hydrogen storage alloys using yttrium (Y) as a rare earth element mixed with La and Ni are also listed as reference examples.
この本発明の組成の水素吸蔵合金と比較例として、以
下に記す水素吸蔵合金を得た。As a hydrogen storage alloy having the composition of the present invention and a comparative example, the following hydrogen storage alloy was obtained.
比較例１ 実施例１と同様にして、所定量のLa,Nd,Niの粉末混合
体をプレスした後、アルゴンアーク溶解炉にてこれを溶
解し、第１表の比較例Ｇ〜Ｉに示す公知の水素吸蔵合金
（特開昭60−197835号公報に示される）の組成を持つボ
タン状合金鋳塊を得た。なお、ここで用いた合金材料を
もいずれも99.9％の純度を持つものである。Comparative Example 1 After pressing a predetermined amount of a La, Nd, Ni powder mixture in the same manner as in Example 1, the powder mixture was melted in an argon arc melting furnace, and shown in Comparative Examples GI of Table 1. A button-shaped alloy ingot having a composition of a known hydrogen storage alloy (shown in JP-A-60-197835) was obtained. The alloy materials used here all have a purity of 99.9%.
以上のようにして得た実施例１のＤ〜Ｆに係る合金鋳
塊、参考例Ａ〜Ｃに係る金属塊ならびに比較例１に係る
合金鋳塊を、100メッシュ程度に粉砕し、水素化平衡特
性試験、及び水素吸収・放出サイクル特性試験に供し
た。これらの試験に先立ち、活性化処理を行ったとこ
ろ、いずれの合金も80℃の真空排気及び常温での10atm
の水素加圧により水素吸収を開始した。The alloy ingots according to D to F, the metal ingots according to Reference Examples A to C, and the alloy ingot according to Comparative Example 1 obtained in the above manner were pulverized to about 100 mesh, and hydrogenation equilibrium was obtained. It was subjected to a characteristic test and a hydrogen absorption / desorption cycle characteristic test. Prior to these tests, activation treatment was performed.Each alloy was evacuated to 80 ° C and 10atm at room temperature.
Hydrogen absorption was started by pressurizing hydrogen.
水素化平衡特性試験は、公知のジーベルツ装置を用い
た圧力−水素吸収量等温線図の測定により行った。以上
の特性試験の結果をまとめて、第１表に示す。The hydrogenation equilibrium property test was performed by measuring a pressure-hydrogen absorption amount isotherm diagram using a known Siebeltz apparatus. Table 1 summarizes the results of the above characteristic tests.
同表より、本発明の実施例１に係る水素吸蔵合金は、
比較例１に示す公知のものに比べて、同一平衡圧力での
HSファクターが約1/3であり、その値が1.0以下であるこ
とが分かる。From the table, the hydrogen storage alloy according to the first embodiment of the present invention,
Compared to the known one shown in Comparative Example 1,
It can be seen that the HS factor is about 1/3 and its value is 1.0 or less.
但し、第１表において、HSファクターは、0.9wt％の
水素を可逆的に吸蔵放出するための圧力の自然対数差を
示す。 However, in Table 1, the HS factor indicates the natural logarithm of the pressure for reversibly occluding and releasing 0.9 wt% of hydrogen.
そして、実施例１に係るＤ〜Ｆの組成の本発明水素吸
蔵合金によれば、熱駆動型冷凍システムに必要な平衡圧
力（20〜35℃で約10atm）と、HSファクター（1.0以下）
を満足するが、比較例１のＧ〜Ｉに係る水素吸蔵合金で
は、平衡圧力、HSファクターはどちらか一方しか満足で
きないことが認められる。Then, according to the hydrogen storage alloy of the present invention having the composition of D to F according to Example 1, the equilibrium pressure (about 10 atm at 20 to 35 ° C.) required for the heat driven refrigeration system and the HS factor (1.0 or less)
However, in the hydrogen storage alloys according to GI of Comparative Example 1, only one of the equilibrium pressure and the HS factor can be satisfied.
以上のように、本発明の水素吸蔵合金は、熱駆動型冷
凍システムに対して要求される比較的高い平衡水素圧力
（20〜35℃で約10atm）、優れたHSファクター（1.0以
下）を兼ね備えた優れた特性を持つ。As described above, the hydrogen storage alloy of the present invention has a relatively high equilibrium hydrogen pressure (about 10 atm at 20 to 35 ° C.) and an excellent HS factor (1.0 or less) required for a heat driven refrigeration system. With excellent properties.
尚、参考例として挙げたＡの組成の合金（La0.74Ｙ
0.26Ni5）の20℃における平衡水素圧力と水素吸収量
を、従来合金（La0.5Nd0.5Ni5）と比較したものを、第
１図に示すこととした。同グラフからは、La0.74Nd0.26
Ni5の合金（参考例合金）は、La0.5Nd0.5Ni5の合金（従
来合金）に比較して、ヒステリシスあるいはプラトー部
の傾斜が小さく、可逆的に水素を吸蔵・放出するための
圧力差が小さくなっていることが理解されるであろう。Incidentally, an alloy having the composition of A (La 0.74 Y
FIG. 1 shows a comparison of the equilibrium hydrogen pressure and the hydrogen absorption of 0.26 Ni 5 ) at 20 ° C. with the conventional alloy (La 0.5 Nd 0.5 Ni 5 ). The graph shows that La 0.74 Nd 0.26
The Ni 5 alloy (reference alloy) has a smaller hysteresis or plateau slope than the La 0.5 Nd 0.5 Ni 5 alloy (conventional alloy), and the pressure difference for reversibly occluding and releasing hydrogen. Will be understood to be smaller.
また、本発明の水素吸蔵合金の実施例１（NoD,E,F）
と比較例１（NoG,H,I）に係るLa1-xNdxNi5合金における
Laに対するNdの置換量（Ｘ）とHSファクターの関係を第
２図に示す。Example 1 of the hydrogen storage alloy of the present invention (NoD, E, F)
And La 1-x Nd x Ni 5 alloy according to Comparative Example 1 (NoG, H, I)
FIG. 2 shows the relationship between the substitution amount (X) of Nd for La and the HS factor.
第２図より、本発明の実施例１（NoD,E,F）に係る水
素吸蔵合金は、所望の平衡水素圧力（20〜35℃で約10at
m）を得るための置換量の範囲内で、HSファクターが、
0.1以下であることが認められるが、比較例１に係る水
素吸蔵合金は、比較的高い平衡水素圧力（20〜35℃で約
10atm）では、HSファクターが、1.0以上であることが分
かる。From FIG. 2, it can be seen that the hydrogen storage alloy according to Example 1 (NoD, E, F) of the present invention has a desired equilibrium hydrogen pressure (about 10 at
m) within the range of substitution to obtain
The hydrogen storage alloy according to Comparative Example 1 has a relatively high equilibrium hydrogen pressure (about 20 to 35 ° C.).
10atm), it can be seen that the HS factor is 1.0 or more.
（ト）発明の効果 以上、説明したように、本発明の組成の水素吸蔵合金
により、熱駆動型冷凍システムに対して要求される比較
的高い平衡水素圧力（20〜35℃で約10atm）と、優れたH
Sファクター（1.0以下）を兼ね備えることができる。こ
れにより、実用的な熱駆動型冷凍システムの構築が可能
となり、水素エネルギーシステムの要素技術の確立に対
する寄与は極めて大きいものとなる。(G) Effect of the Invention As described above, the hydrogen storage alloy having the composition of the present invention can achieve a relatively high equilibrium hydrogen pressure (about 10 atm at 20 to 35 ° C.) required for a heat driven refrigeration system. Excellent H
It can have S factor (1.0 or less). This makes it possible to construct a practically heat-driven refrigeration system, and greatly contributes to the establishment of the elemental technology of the hydrogen energy system.
第１図は、第１表のNo.Aに示す参考例としての水素吸蔵
合金（La0.74Ｙ0.26Ni5）と比較例１に係る従来の水素
吸蔵合金（La0.5Nd0.5Ni5）合金との平衡水素圧力と水
素吸蔵合金との関係を示す特性図である。第２図は、本
発明の水素吸蔵合金と比較例に係るLa1-xMxNi5（m;Sm,N
d）合金におけるLaに対するＭの置換量（ｘ）とHSファ
クターの関係を示す図である。FIG. 1 shows a hydrogen storage alloy (La 0.74 Y 0.26 Ni 5 ) as a reference example shown in No. A of Table 1 and a conventional hydrogen storage alloy (La 0.5 Nd 0.5 Ni 5 ) alloy according to Comparative Example 1. FIG. 3 is a characteristic diagram showing a relationship between an equilibrium hydrogen pressure and a hydrogen storage alloy. FIG. 2 shows the hydrogen storage alloy of the present invention and La 1-x MxNi 5 (m; Sm, N
d) A diagram showing the relationship between the substitution amount (x) of M for La in the alloy and the HS factor.
───────────────────────────────────────────────────── フロントページの続き (72)発明者 齋藤 俊彦 大阪府守口市京阪本通２丁目18番地 三 洋電機株式会社内 (56)参考文献 特開 平２−291665（ＪＰ，Ａ) (58)調査した分野(Int.Cl.6，ＤＢ名) C22C 19/00──────────────────────────────────────────────────続 き Continuation of the front page (72) Inventor Toshihiko Saito 2-18-18 Keihanhondori, Moriguchi-shi, Osaka Sanyo Electric Co., Ltd. (56) References JP-A-2-291665 (JP, A) (58) Field surveyed (Int. Cl. 6 , DB name) C22C 19/00
Claims (1)
表されることを特徴とする水素吸蔵合金。1. A hydrogen storage alloy represented by the following general formula: La 1-x Sm x Ni 5 (0.4 ≦ X ≦ 0.55).
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2107458A JP2794477B2 (en) | 1990-04-25 | 1990-04-25 | Hydrogen storage alloy |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP2107458A JP2794477B2 (en) | 1990-04-25 | 1990-04-25 | Hydrogen storage alloy |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH046236A JPH046236A (en) | 1992-01-10 |
| JP2794477B2 true JP2794477B2 (en) | 1998-09-03 |
Family
ID=14459686
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP2107458A Expired - Fee Related JP2794477B2 (en) | 1990-04-25 | 1990-04-25 | Hydrogen storage alloy |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP2794477B2 (en) |
Families Citing this family (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| EP4209608B1 (en) | 2020-09-01 | 2025-06-04 | Santoku Corporation | Hydrogen storage material, hydrogen storage container and hydrogen supply apparatus |
| CN112708801B (en) * | 2020-12-03 | 2022-04-22 | 包头稀土研究院 | Single-phase PuNi3Preparation method of type superlattice La-Y-Ni hydrogen storage alloy |
Family Cites Families (1)
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|---|---|---|---|---|
| JP3345889B2 (en) * | 1989-02-23 | 2002-11-18 | 松下電器産業株式会社 | Manufacturing method of alkaline storage battery and its negative electrode |
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1990
- 1990-04-25 JP JP2107458A patent/JP2794477B2/en not_active Expired - Fee Related
Also Published As
| Publication number | Publication date |
|---|---|
| JPH046236A (en) | 1992-01-10 |
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