JPH1025531A - Positive electrode vessel material made of cobalt-base alloy for sodium-sulfur battery - Google Patents

Positive electrode vessel material made of cobalt-base alloy for sodium-sulfur battery

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Publication number
JPH1025531A
JPH1025531A JP18445296A JP18445296A JPH1025531A JP H1025531 A JPH1025531 A JP H1025531A JP 18445296 A JP18445296 A JP 18445296A JP 18445296 A JP18445296 A JP 18445296A JP H1025531 A JPH1025531 A JP H1025531A
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na
positive electrode
content
sodium
base alloy
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JP18445296A
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Japanese (ja)
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Hiroaki Kikuchi
弘明 菊池
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Mitsubishi Materials Corp
三菱マテリアル株式会社
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    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies or technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage
    • Y02E60/12Battery technologies with an indirect contribution to GHG emissions mitigation

Abstract

PROBLEM TO BE SOLVED: To provide a positive electrode vessel material made of Co-base alloy for Na-S battery, having high strength and excellent corrosion resistance to Na and S. SOLUTION: A positive electrode vessel 3 material for Na-S battery is constituted of a Co-base alloy which has a composition consisting of, by weight, 15-30% Cr, 5-30% Ni, 10-20% W, 0.1-5% Fe, 0.2-2% Mn, 0.01-0.3% C, and the balance >=35% Co with inevitable impurities and further containing, if necessary, 0.01-0.2% La.

Description

【発明の詳細な説明】 DETAILED DESCRIPTION OF THE INVENTION

【0001】 [0001]

【発明の属する技術分野】この発明は、高強度を有し、 BACKGROUND OF THE INVENTION The present invention has a high strength,
かつ溶融多硫化ナトリウムおよび溶融硫黄(S)に対する耐食性(以下、耐Na・S腐食性と云う)にすぐれ、 And corrosion resistance to molten sodium polysulfide and molten sulfur (S) (hereinafter, referred to as anti-Na · S corrosive) to excellent,
したがってナトリウム(Na)−硫黄(S)電池の大容量化および軽量化に寄与するCo基合金製正極容器材に関するものである。 Sodium Therefore (Na) - relates sulfur (S) contributes Co-based alloy cathode container material in the mass and weight of the battery.

【0002】 [0002]

【従来の技術】従来、一般に、Na−S電池が、電気自動車や電力貯蔵などに用いられ、さらに図1にその1例を概略縦断面図で示す通り、一端が閉じたβ−アルミナ製固体電解質管(1)の開口端にα−アルミナ製絶縁リング(2)をガラスで封着し、この絶縁リング(2)に正極容器(3)と負極棒(4)を、前記固体電解質管内にはNa(5)を、またこれと前記正極容器との空隙にはS(6)を充填した状態で、それぞれ封着した構造をもつことが知られている。 Conventionally, in general, Na-S cells, used in electric vehicles and power storage, as shown further the example in schematic longitudinal sectional view in FIG. 1, closed at one end β- alumina solid open end α- alumina insulating ring of the electrolyte tube (1) and (2) sealed with glass, the Fukyokubo (4) and the positive electrode container (3) in the insulating ring (2), to said solid electrolyte tube in the state in the gap filled with S (6) of the positive electrode container Na (5), also with this, it is known to have a sealed structure, respectively. また、上記の構造を有するN Further, N having the above structure
a−S電池においては、一般に動作温度が350℃であり、放電時には溶融NaがNaイオンになり固体電解質管1の中を正極容器3側に移動して、溶融Sと反応して多硫化ナトリウムを生成し、一方充電はこの逆反応となるものである。 In a-S cells, generally the operating temperature is 350 ° C., during discharging molten Na moves through the solid electrolyte tube 1 becomes Na ions in the positive electrode container 3 side, sodium polysulfide reacts with the molten S It generates, whereas charging and serves as a reverse reaction. したがって、Na−S電池の正極容器は、腐食性の強い多硫化ナトリウムおよび溶融Sにさらされる苛酷な腐食環境下におかれるため、耐Na・S腐食性の良好な、例えば特開平7−85886号公報に記載されるようなFe−Cr系合金、すなわち、重量%で(以下、%はいずれも重量%を示す)、 Cr:25〜40%、 Mo:1〜3.5%、 Al:0.5〜3.5%、 を含有し、残りがFeと不可避不純物からなる組成を有するFe−Cr系合金などが用いられている。 Thus, the positive electrode container Na-S cells, because they are placed under severe corrosive environments exposed to strong corrosive sodium polysulfide and melt S, anti-Na · S corrosive good, for example, JP-A-7-85886 Fe-Cr-based alloy as described in JP, i.e., in weight% (hereinafter,% is also shown by weight% one can), Cr: 25~40%, Mo: 1~3.5%, Al: 0.5 to 3.5 percent, contain, etc. Fe-Cr-based alloy having a composition balance being Fe and inevitable impurities is used.

【0003】 [0003]

【発明が解決しようとする課題】一方、近年の無公害エネルギーの益々の必要性から、Na−S電池が注目され、かつこれの大容量化および軽量化が強く求められているが、これらの要求を満足させる手段の1つとして正極容器の薄肉化がある。 [Problems that the Invention is to Solve Meanwhile, the increasing need for modern pollution-free energy, Na-S cell has attracted attention, and has a large capacity and weight of which is a strong demand, these one means to satisfy the request is thinner positive electrode container. しかしながら、上記の従来正極容器を構成するFe−Cr系合金はじめ、その他の材料は充分な強度と耐Na・S腐食性を具備するものでないために、これを薄肉化することは実用上困難であるのが現状である。 However, Fe-Cr-based alloy began constitute prior positive electrode container of the above, for other materials are not intended to comprise a sufficient strength and resistance to Na · S corrosive, it is practically difficult to thin it there's at present.

【0004】 [0004]

【課題を解決するための手段】そこで、本発明者等は、 Means for Solving the Problems] The present inventors have
上述のような観点から、より一段と高い強度を有し、かつ耐Na・S腐食性にもすぐれたNa−S電池の正極容器を開発すべく研究を行った結果、 Na−S電池の正極容器を、 Cr:15〜30%、 Ni:5〜30%、 W:10〜20%、 Fe:0.1〜5%、 Mn:0.2〜2%、 C:0.01〜0.3%、 を含有し、さらに必要に応じて、 La:0.01〜0.2%、 を含有し、残りがCo(但し35%以上含有)と不可避不純物からなる組成を有するCo基合金で構成すると、 From the viewpoint as described above, more much higher strength have, and results to conducted research to develop a positive electrode container of Na-S battery excellent in resistance to Na · S corrosive, the positive electrode container Na-S battery the, Cr: 15~30%, Ni: 5~30%, W: 10~20%, Fe: 0.1~5%, Mn: 0.2~2%, C: 0.01~0.3 %, and containing, if necessary, La: 0.01 to 0.2%, contains, consists of a Co-based alloy having a composition balance being Co (provided that 35% or more content) and unavoidable impurities Then,
この結果のCo基合金製正極容器材は、高強度とすぐれた耐Na・S腐食性をもつことから、これを薄肉化してもNa−S電池への実用に際して充分満足な性能を長期に亘って発揮するという研究結果を得たのである。 Co-based alloy cathode container material for this result is over because of its superior resistance to Na · S corrosive and high strength, which a satisfactory performance in long-term practical use of even thinned to Na-S battery than it was to obtain the results of a study that demonstrated Te.

【0005】この発明は、上記の研究結果に基づいてなされたものであって、 Cr:15〜30%、 Ni:5〜30%、 W:10〜20%、 Fe:0.1〜5%、 Mn:0.2〜2%、 C:0.01〜0.3%、 を含有し、さらに必要に応じて、 La:0.01〜0.2%、 を含有し、残りがCo(但し35%以上含有)と不可避不純物からなる組成を有するCo基合金で構成してなる、高強度およびすぐれた耐Na・S腐食性を有するN [0005] This invention was made based on the above findings, Cr: 15~30%, Ni: 5~30%, W: 10~20%, Fe: 0.1~5% , Mn: 0.2~2%, C: 0.01~0.3%, containing, if necessary, La: 0.01 to 0.2%, containing, remainder Co ( However consisting constituted by Co-based alloy having a composition 35% or more content) and unavoidable impurities, N having a high strength and excellent resistance to Na · S corrosive
a−S電池のCo基合金製正極容器材に特徴を有するものである。 Those characterized by a Co-based alloy cathode container material a-S cells.

【0006】つぎに、この発明の正極容器材を構成するCo基合金の組成を上記の通りに限定した理由を説明する。 [0006] Next, the reasons for limiting the composition of the Co-based alloy forming the positive electrode container material of the present invention as described above. (a)Cr Cr成分には、素地に固溶して耐Na・S腐食性を向上させると共に、素地に微細に分散する炭化物を形成して強度を向上させる作用があるが、その含有量が15%未満では前記作用に所望の向上効果が得られず、一方その含有量が30%を越えると、圧延加工性および溶接性が低下(いずれの場合も割れが発生するようになる)するようになることから、その含有量を15〜30%、望ましくは20〜24%と定めた。 The (a) Cr Cr component, a solid solution in the matrix improves the resistance to Na · S corrosive, but an effect of improving the strength by forming a finely dispersed carbides in the matrix, its content in less than 15% can not be obtained the desired improvement in the working, whereas when the content exceeds 30%, the rolling workability and weldability (so even cracking occur cases) decreased to as from becoming, the content of 15% to 30%, preferably defined as 20-24%.

【0007】(b)Ni Ni成分には、素地に固溶して強度を向上させる作用があるが、その含有量が5%未満では所望の強度向上効果が得られず、一方その含有量が30%を超えると、耐N [0007] (b) Ni Ni component, it has an effect of improving the strength as a solid solution in the matrix, its content is less than 5% can not be obtained the desired effect of improving strength, while its content When more than 30%, resistance to N
a・S腐食性が低下するようになることから、その含有量を5〜30%、望ましくは20〜25%と定めた Since a · S corrosion resistance will be lowered, the content of 5-30%, preferably defined as 20-25%

【0008】(c)W W成分には、素地に固溶し、かつ素地中に微細に分散する炭化物を形成して強度を向上させる作用があるが、その含有量が10%未満では前記作用に所望の向上効果が得られず、一方その含有量が20%を越えると、圧延加工性が低下するようになることから、その含有量を10 [0008] (c) W W component dissolves into the matrix, and it has the effect of improving the strength by forming a finely dispersed carbides in the matrix, the content of the working is less than 10% not obtained the desired improvement in, whereas when the content exceeds 20%, since the rolling resistance will be lowered, the content 10
〜20%、望ましくは13〜16%と定めた。 20%, preferably defined as 13-16%.

【0009】(d)Fe Fe成分には、素地に固溶して圧延加工性を向上させる作用があるが、その含有量が0.1%未満では前記作用に所望の向上効果が得られず、一方その含有量が5%を越えると耐Na・S腐食性が低下するようになることから、その含有量を0.1〜5%、望ましくは0.1〜3 [0009] The (d) Fe Fe component, there is an effect of improving rolling resistance by solid solution in the matrix, the content can not be obtained the desired improvement in the working is less than 0.1% , whereas since the content thereof is resistant Na · S corrosive exceeds 5% will reduce, the content of 0.1% to 5%, preferably 0.1 to 3
%と定めた。 % As determined.

【0010】(e)Mn Mn成分には、素地に固溶して、耐Na・S腐食性を向上させる作用があるが、その含有量が0.2%未満では前記作用に所望の効果が得られず、一方その含有量が2 [0010] The (e) Mn Mn component, a solid solution in the matrix, but an effect of improving the anti-Na · S corrosive, its content is desired effect on the action is less than 0.2% not obtained, while its content is 2
%を越えると、素地にフェライト相が出現するようになって耐Na・S腐食性に低下傾向が現れるようになることから、その含有量を0.2〜2%、望ましくは0.2 % By weight, from becoming so ferrite phase appears to appear decline in resistance to Na · S corrosive matrix, the content of 0.2 to 2 percent, preferably 0.2
〜1.3%と定めた。 It was defined as 1.3%.

【0011】(f)C C成分には、素地に固溶して、これを固溶強化するほか、CrおよびWと結合して炭化物を形成し、もって強度を向上させる作用があるが、その含有量が0.01% [0011] (f) C C component is dissolved in the matrix, in addition to solid solution strengthening this combines with Cr and W form carbides, but an effect of improving the strength with its content of 0.01%
未満では前記作用に所望の向上効果が得られず、一方その含有量が0.3%を越えると、圧延加工性が低下するようになることから、その含有量を0.01〜0.3 Not obtained the desired improvement in the working is less than, whereas when the content exceeds 0.3%, since the rolling resistance will be lowered, the content of 0.01 to 0.3
%、望ましくは0.05〜0.15%と定めた。 %, Preferably defined as 0.05 to 0.15 percent.

【0012】(g)La La成分には、耐Na・S腐食性を一段と向上させる作用があるので、必要に応じて含有されるが、その含有量が0.01%未満では所望の向上効果が得られず、一方その含有量が0.2%を越えると酸化物が生成するようになって強度が低下するようになるないことから、その含有量を0.01〜0.2%、望ましくは0.03〜 [0012] (g) La La in component, there is a function to further improve the resistance to Na · S corrosive, but are contained as necessary, improved its content desired is less than 0.01%, the effect can not be obtained, whereas since there is no so the strength adapted to generate oxides exceeds 0.2% decrease its content, its content 0.01 to 0.2%, preferably 0.03
0.12%と定めた。 It was defined as 0.12%.

【0013】(h)Co Co成分は、すぐれた耐Na・S腐食性を確保するのに不可欠の成分であり、したがってその含有量が35%未満では所望の耐Na・S腐食性が得られないことから、 [0013] (h) Co Co component is an essential component to ensure excellent resistance to Na · S corrosive, therefore the content thereof to obtain desired anti-Na · S corrosive is less than 35% since it is not,
その含有量を35%以上と定めた。 The content was defined as 35% or more.

【0014】 [0014]

【発明の実施の形態】つぎに、この発明の正極容器材を実施例により具体的に説明する。 DESCRIPTION OF THE PREFERRED EMBODIMENTS Next, specifically described by the positive electrode container material embodiment of the present invention. 原料として金属Co、 Metal Co as a raw material,
テルミットクロム、金属W、Fe−Ni合金、炭素粉末、電解Ni、Ni−La合金、および金属Mnを用い、これら原料を所定の割合に配合し、これを高周波誘導溶解炉にて脱酸剤としてSiおよびAlを用いて溶解して、それぞれ表1、2に示される成分組成をもった溶湯を調製し、この溶湯をさらに同じく脱酸剤としてNi Thermite chromium, W, Fe-Ni alloy, carbon powder, electrolytic Ni, Ni-La alloy, and a metal Mn, are blended raw material in a predetermined ratio, this as a deoxidizer in an induction furnace was dissolved with Si and Al, the melt having a chemical composition which is respectively shown in tables 1 and 2 were prepared, Ni as further likewise deoxidizing agent this melt
−Mg合金を用いて脱酸した状態で出湯して、外径:5 And tapping while deoxidized with -Mg alloy, outer diameter: 5
00mmのインゴットに鋳造し(この結果インゴットは通常0.1〜0.6%のSi、0.1〜0.4%のA And cast into ingots of 300 mm (The result ingot is usually 0.1 to 0.6% of Si, 0.1 to 0.4% of the A
l、および0.01〜0.06%のMgを含有するようになる)、前記インゴットを1180℃に10時間保持の条件で均質化処理した後、1100〜1200℃の温度で熱間圧延して厚さ:3mmの熱延板とし、さらにこの熱延板に冷間圧延を施して厚さ:0.5mmの冷延板とすることにより本発明正極容器材1〜17および従来正極容器材を製造した。 l, and so contains from .01 to 0.06% of Mg), it was homogenized under the conditions of holding 10 hours the ingot to 1180 ° C., hot rolled at a temperature of 1100 to 1200 ° C. Te thickness: a 3mm hot rolled sheet, still the hot-rolled sheet thickness by performing cold rolling of: the present invention by a 0.5mm cold rolled sheet positive electrode container material 1 to 17 and a conventional positive electrode container material It was prepared.

【0015】ついで、この結果得られた各種の正極容器材より、強度を評価する目的で、平行部長さ:120m [0015] Then, from the resulting various cathode container material, the purpose of evaluating the strength, parallel portion length: 120 m
m×幅:20mm×厚さ:0.5mmの寸法をもった引張試験片を切り出し、さらにこれらの耐Na・S腐食性を評価する目的で、造管機とTIG溶接機を用いて、外径:65mm×長さ:400mmの寸法をもった管体を形成し、これに1180℃に30分間保持後水冷の条件で固溶化熱処理を施すことによりNa−S電池の正極容器を形成した。 m × width: 20 mm × thickness: cut out 0.5mm tensile specimen dimensions with the further the purpose of evaluating these resistant Na · S corrosive, with pipe making machine and TIG welding machine, an outer diameter: 65 mm × length: 400 mm size to form a tubular body having a, to form a positive electrode container of Na-S battery by performing solution treatment at 30 minute hold after water-cooling conditions to 1180 ° C. thereto. 引張試験は、350℃で行って引張強さを測定し、また上記正極容器については、Na−S電池に組み込んで、運転温度:350℃、充電電流密度:2 Tensile test measures the tensile strength performed at 350 ° C., also for the positive electrode container, incorporated into Na-S battery, operating temperature: 350 ° C., charging current density: 2
30mA/cm 2 、放電電流密度:300mA/cm 30 mA / cm 2, discharge current density: 300 mA / cm
2 、連続充放電回数:150サイクルの加速条件で実機試験を行い、正極容器内面における最大浸食深さを測定した。 2, the continuous charge and discharge count: perform physical testing under accelerated conditions of 150 cycles was measured maximum erosion depth in the cathode inner surface of the container. これらの測定結果を表1、2に示した。 These measurement results are shown in Tables 1 and 2.

【0016】 [0016]

【表1】 [Table 1]

【0017】 [0017]

【表2】 [Table 2]

【0018】 [0018]

【発明の効果】表1、2に示される結果から、本発明正極容器材1〜17は、いずれも従来正極容器材に比して高強度を有すると共に、一段とすぐれた耐Na・S腐食性を示すことが明らかである。 From the results shown in Tables 1 and 2 according to the present invention, the present invention positive electrode container material 1 to 17, both with a high strength in comparison with the conventional cathode container material, more excellent resistance to Na · S corrosive the it is clear that the show. 上述のように、この発明のCo基合金製正極容器材は、高強度とすぐれた耐Na As described above, Co-based alloy cathode container material of the present invention, anti-Na with excellent high strength
・S腐食性を具備しているので、これを薄肉化した状態で実用に供することが可能であることから、Na−S電池の大容量化および軽量化に寄与かることができるなど工業上有用な特性を有するのである。 Since · S is provided with a corrosive industrial utility such as this because it is for practical use while thin, can hunt contributes to a large capacity and weight of the Na-S battery than it has the characteristics.

【図面の簡単な説明】 BRIEF DESCRIPTION OF THE DRAWINGS

【図1】Na−S電池の構造を例示する概略縦断面図である。 1 is a schematic longitudinal sectional view illustrating the structure of Na-S battery.

【符号の説明】 DESCRIPTION OF SYMBOLS

1 固体電解質管 2 絶縁リング 3 正極容器 4 負極棒 5 Na 6 S 1 solid electrolyte tube 2 insulating ring 3 positive vessel 4 Fukyokubo 5 Na 6 S

Claims (2)

    【特許請求の範囲】 [The claims]
  1. 【請求項1】 重量%で、 Cr:15〜30%、 Ni:5〜30%、 W:10〜20%、 Fe:0.1〜5%、 Mn:0.2〜2%、 C:0.01〜0.3%、 を含有し、残りがCo(但し35%以上含有)と不可避不純物からなる組成を有するCo基合金で構成したことを特徴とするナトリウム−硫黄電池のCo基合金製正極容器材。 1. A weight%, Cr: 15~30%, Ni: 5~30%, W: 10~20%, Fe: 0.1~5%, Mn: 0.2~2%, C: from 0.01 to 0.3 percent, contain sodium, characterized in that the rest is composed of Co-based alloy having a composition consisting of incidental impurities and Co (although containing more than 35%) - Co-based alloy sulfur battery manufacturing the positive electrode container material.
  2. 【請求項2】 重量%で、 Cr:15〜30%、 Ni:5〜30%、 W:10〜20%、 Fe:0.1〜5%、 Mn:0.2〜2%、 C:0.01〜0.3%、 を含有し、さらに、 La:0.01〜0.2%、 を含有し、残りがCo(但し35%以上含有)と不可避不純物からなる組成を有するCo基合金で構成したことを特徴とするナトリウム−硫黄電池のCo基合金製正極容器材。 2. A weight%, Cr: 15~30%, Ni: 5~30%, W: 10~20%, Fe: 0.1~5%, Mn: 0.2~2%, C: 0.01 to 0.3 percent, contain further, La: 0.01 to 0.2% containing, Co group having the composition balance being Co (provided that 35% or more content) and unavoidable impurities sodium characterized by being composed of an alloy - Co based alloy cathode container material sulfur battery.
JP18445296A 1996-07-15 1996-07-15 Positive electrode vessel material made of cobalt-base alloy for sodium-sulfur battery Pending JPH1025531A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2000251898A (en) * 1999-02-25 2000-09-14 Wilson Greatbatch Ltd Cobalt-based alloy as positive electrode current collector in nonaqueous electrochemical battery

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2000251898A (en) * 1999-02-25 2000-09-14 Wilson Greatbatch Ltd Cobalt-based alloy as positive electrode current collector in nonaqueous electrochemical battery

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