JP3704241B2 - Joining structure of insulating ring and anode cylindrical fitting in sodium-sulfur battery - Google Patents

Joining structure of insulating ring and anode cylindrical fitting in sodium-sulfur battery Download PDF

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Publication number
JP3704241B2
JP3704241B2 JP26349798A JP26349798A JP3704241B2 JP 3704241 B2 JP3704241 B2 JP 3704241B2 JP 26349798 A JP26349798 A JP 26349798A JP 26349798 A JP26349798 A JP 26349798A JP 3704241 B2 JP3704241 B2 JP 3704241B2
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Prior art keywords
insulating ring
anode
sodium
cylindrical
fitting
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JP2000090967A (en
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光広 庄村
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NGK Insulators Ltd
Tokyo Electric Power Co Inc
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NGK Insulators Ltd
Tokyo Electric Power Co Inc
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    • 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
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    • Y02E60/10—Energy storage using batteries

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Description

【０００１】
【発明の属する技術分野】
本発明は、ナトリウム−硫黄電池における絶縁リングと陽極筒状金具との接合構造に係り、特に、電池昇降温時に固体電解質管と陽極容器との熱収縮膨張差により生じる荷重に対する、絶縁リングと陽極筒状金具との接合部の強度信頼性を向上することができる接合構造に関する。
【０００２】
【従来の技術】
ナトリウム−硫黄電池は、一方に陰極活性物質である溶融金属ナトリウム、他方には陽極活性物質である溶融硫黄を配し、両者をナトリウムイオンに対して選択的な透過性を有するβ−アルミナ固体電解質で隔離し、３００〜３５０℃で作動させる高温二次電池である。
【０００３】
このようなナトリウム−硫黄電池の構造は、例えば図２に示すように、カーボンフェルト等に含浸された溶融硫黄Ｓを収容する円筒状の陽極容器１と、溶融金属ナトリウムＮａを収容するカートリッジ（ナトリウム保護管）６と、このカートリッジ６を内部に収納し、ナトリウムイオンＮａ+を選択的に透過させる機能を有する有底円筒状の固体電解質管５と、カートリッジ６と固体電解質管５の間の間隙部に、そのカートリッジ６及び固体電解質管５からそれぞれ所定の間隔をおいて配設された有底円筒状の隔壁管１１とからなる。
【０００４】
固体電解質管５はその開口端にガラス接合されたα−アルミナ製の絶縁リング４及び陽極筒状金具３を介して陽極容器１と結合されている。また、絶縁リング４の上端面には陰極金具８が熱圧接合され、この陰極金具８に陰極蓋９が溶接固定されている。陽極容器１の外周上部と陰極蓋９の上面には、それぞれ陽極側端子２と陰極側端子１０が設けられている。カートリッジ６の上部空間には、窒素ガスやアルゴンガス等の不活性ガスＧが所定の圧力で封入され、この不活性ガスＧによりカートリッジ６内のナトリウムＮａがカートリッジ底部に設けられた小孔７から流出する方向へ加圧されている。
【０００５】
かかる構造を有するナトリウム−硫黄電池において、放電時にはカートリッジ６の小孔７から供給されるナトリウムＮａが、隔壁管１１とカートリッジ６との間隙内で上方に移動した後、隔壁管１１の上端を乗り越えて、隔壁管１１と固体電解質管５との間隙内で下方に移動し、更に、固体電解質管５をナトリウムイオンとなって透過して、陽極容器１内の硫黄Ｓ及び外部回路を通ってきた電子と反応し多硫化ナトリウムを生成する。充電時には放電とは逆にナトリウム及び硫黄の生成反応が起こる。
【０００６】
図３は、このような従来のナトリウム−硫黄電池における絶縁リングと陽極筒状金具との接合構造を示す要部断面図である。陽極筒状金具３は、円筒部３ａと円筒部３ａ下端から円筒部３ａの内部方向に張り出したフランジ部３ｂとを有する。絶縁リング４は、この陽極筒状金具３の円筒部３ａ内に挿入され、金属ロウ材等の接合材１２を介して、フランジ部３ｂの上面と絶縁リング４の下端面とが熱圧接合されている。
【０００７】
ここで、陽極筒状金具３の円筒部３ａ内への絶縁リング４の挿入については、円筒部３ａの内周面と絶縁リング４の外周面とのクリアランス１３の値Ｃが大きい方が作業が容易であり、特に大量生産や組立作業の自動化等を考慮した場合に好ましい。ただし、このクリアランス１３の値Ｃが大きすぎる場合には、芯ズレ等の問題が生じるので、従来はクリアランス１３の値Ｃを１ｍｍ程度となるように設定していた。
【０００８】
ところで、ナトリウム−硫黄電池は、電池作動時と停止時の間に温度差があり、停止時の低温状態においては、多硫化ナトリウム又は硫黄が固化し、固体電解質管５と陽極容器１とは相互に拘束することになる。そして、電池降温時には、固体電解質管５及び陽極容器１はともに熱収縮するが、金属である陽極容器１の熱収縮は大きく、この陽極容器１の収縮が熱収縮の小さい固体電解質管５に抑制されるため、固体電解質管５と陽極容器１とを結合させている絶縁リング４と陽極筒状金具３との接合部に下方への荷重が働く（図３の矢印方向）。
【０００９】
そこで、従来においては、この荷重に起因する絶縁リング４と陽極筒状金具３の接合部の破損を防止するため、陽極容器１の周面の一部に軸方向に収縮する内周面方向へのくびれを形成してバネ効果を持たせ、荷重を低減する等の対策が行われていた。
【００１０】
【発明が解決しようとする課題】
しかしながら、上記のような対策を施した場合であっても、絶縁リング４の陽極筒状金具３との結合端部が強度的に弱かったりすると割れが生じることがあり、また、この問題はナトリウム−硫黄電池の大型化が進むにつれより一層顕著になってきている。
【００１１】
本発明は、このような状況に鑑みてなされたものであり、その目的とするところは、電池降温時の固体電解質管と陽極容器との熱収縮差により生じる荷重に対する、絶縁リングと陽極筒状金具との結合部の強度信頼性を向上し、結合部の損傷を防止することができる接合構造を提供することにある。
【００１２】
【課題を解決するための手段】
本発明によれば、固体電解質管の開口端に絶縁リングを接合し、当該絶縁リングに、陽極容器と結合した円筒部と当該円筒部下端から当該円筒部の内部方向に張り出したフランジ部とを有する陽極筒状金具を、前記フランジ部の上面が前記絶縁リングの下端面に接合されるように接合材を介して熱圧接合したナトリウム−硫黄電池の絶縁リングと陽極筒状金具との接合構造において、前記陽極筒状金具の円筒部の内周面と、前記絶縁リングの外周面とのクリアランスの値が、０．１５ｍｍ以下であることにより、前記接合材が前記クリアランスの高い位置まで染み上がっていることを特徴とするナトリウム−硫黄電池における絶縁リングと陽極筒状金具との接合構造、が提供される。
【００１３】
【発明の実施の形態】
本発明のナトリウム−硫黄電池における絶縁リングと陽極筒状金具との接合構造においては、図１の要部断面図に示すように、陽極筒状金具３の円筒部３ａの内周面と、絶縁リング４の外周面とのクリアランス１３の値Ｃが、０．１５ｍｍ以下、好ましくは０．０２５〜０．１５ｍｍとなるようにしている。
【００１４】
そして、クリアランス１３の値Ｃをこのように設定したことにより、本発明の接合構造は、このクリアランスの値を１ｍｍ程度に設定していた従来の接合構造に比して、高い接合強度を示す。この理由は定かではないが、クリアランス１３の値Ｃを０．１５ｍｍ以下となるように狭く設定すると、図１のように、陽極筒状金具３と絶縁リング４との熱圧接合の際に、陽極筒状金具３のフランジ部３ｂの上面と絶縁リング４の下端面の間に介在させた金属ロウ材等の接合材１２が、垂直方向に延びるクリアランス１３の高い位置まで染み上がってきて、円筒部３ａの内周面と、絶縁リング４の外周面とを接合し、陽極筒状金具３と絶縁リング４との接合面積が増大するためと考えられる。
【００１５】
なお、上記のように、陽極筒状金具３の円筒部３ａの内周面と絶縁リング４の外周面とのクリアランス１３の値Ｃを、０．１５ｍｍ以下となるように設定した以外、本発明の接合構造は上述の従来の接合構造と変わるところはない。すなわち、従来と同様に、絶縁リング４は、陽極筒状金具３の円筒部３ａ内に挿入され、陽極筒状金具３のフランジ部１３ｂの上面と絶縁リング４の下端面とが、金属ロウ材等の接合材１２を介して熱圧接合される。
【００１６】
【実施例】
以下、本発明を実施例に基づいて更に詳細に説明するが、本発明はこれらの実施例に限定されるものではない。
【００１７】
（実施例）
図１に示す円筒部３ａの内周面と絶縁リング４の外周面とのクリアランス１３の値Ｃが、表１に示すように０．０２５〜０．３ｍｍとなるように種々の寸法で陽極筒状金具３及び絶縁リング４を作製し、それらを熱圧接合して試験片を作製した。こうして作製した各試験片について、図４のように陽極筒状金具３の上部から押し治具２０を介して荷重をかけるとともに、絶縁リング４の下部において受け治具２１により荷重を受けるようにして、陽極筒状金具３と絶縁リング４との接合部の破壊強度を測定した。結果を表１及び図５に示す。
【００１８】
【表１】

Figure 0003704241
【００１９】
表１及び図５に示すとおり、破壊強度はクリアランスの値Ｃが大きくなるにつれて低下しており、当該クリアランスの値Ｃを０．１５ｍｍ以下にすることにより高い接合強度が得られることが判明した。
【００２０】
【発明の効果】
以上説明したように、本発明によれば、絶縁リングと陽極筒状金具との接合部の強度信頼性を向上させることができ、この接合構造を採用することにより、ナトリウム−硫黄電池の信頼性を高めることができる。
【図面の簡単な説明】
【図１】 本発明の接合構造の一実施形態を示す要部断面図である。
【図２】 ナトリウム−硫黄電池の一般的な構造を示す断面図である。
【図３】 従来の接合構造を示す要部断面図である。
【図４】 実施例における接合部の破壊強度の測定法を示す説明図である。
【図５】 実施例の結果を示すグラフである。
【符号の説明】
１…陽極容器、２…陽極側端子、３…陽極筒状金具、４…絶縁リング、５…固体電解質管、６…カートリッジ、７…小孔、８…陰極金具、９…陰極蓋、１０…陰極側端子、１１…隔壁管、１２…接合材、１３…クリアランス。[0001]
BACKGROUND OF THE INVENTION
The present invention relates to a joining structure of an insulating ring and an anode cylindrical metal fitting in a sodium-sulfur battery, and more particularly to an insulating ring and an anode against a load caused by a difference in thermal contraction and expansion between a solid electrolyte tube and an anode container when the battery is heated and lowered. The present invention relates to a joint structure that can improve the strength reliability of a joint portion with a cylindrical metal fitting.
[0002]
[Prior art]
A sodium-sulfur battery is a β-alumina solid electrolyte that has molten metal sodium as a cathode active material on one side and molten sulfur as an anodic active material on the other side, and both have selective permeability to sodium ions. It is a high-temperature secondary battery that is isolated at a temperature of 300 to 350 ° C.
[0003]
For example, as shown in FIG. 2, the structure of such a sodium-sulfur battery includes a cylindrical anode container 1 that contains molten sulfur S impregnated with carbon felt or the like, and a cartridge that contains molten metal sodium Na (sodium). Protective tube) 6, this cartridge 6 is housed inside, and a bottomed cylindrical solid electrolyte tube 5 having a function of selectively permeating sodium ions Na +, and a gap between the cartridge 6 and the solid electrolyte tube 5 And a bottomed cylindrical partition tube 11 disposed at a predetermined distance from the cartridge 6 and the solid electrolyte tube 5.
[0004]
The solid electrolyte tube 5 is coupled to the anode container 1 via an α-alumina insulating ring 4 and an anode cylindrical fitting 3 which are glass-bonded to the open end thereof. A cathode fitting 8 is hot-pressure bonded to the upper end surface of the insulating ring 4, and a cathode lid 9 is welded and fixed to the cathode fitting 8. An anode-side terminal 2 and a cathode-side terminal 10 are provided on the outer periphery of the anode container 1 and the upper surface of the cathode lid 9, respectively. An inert gas G such as nitrogen gas or argon gas is sealed in the upper space of the cartridge 6 at a predetermined pressure, and sodium Na in the cartridge 6 is passed through the small hole 7 provided at the bottom of the cartridge by the inert gas G. Pressurized in the outflow direction.
[0005]
In the sodium-sulfur battery having such a structure, sodium Na supplied from the small hole 7 of the cartridge 6 at the time of discharging moves upward in the gap between the partition tube 11 and the cartridge 6 and then climbs over the upper end of the partition tube 11. Then, it moved downward in the gap between the partition wall tube 11 and the solid electrolyte tube 5, further passed through the solid electrolyte tube 5 as sodium ions, and passed through the sulfur S in the anode container 1 and the external circuit. Reacts with electrons to produce sodium polysulfide. When charging, contrary to discharging, sodium and sulfur are formed.
[0006]
FIG. 3 is a cross-sectional view of a principal part showing a joining structure between an insulating ring and an anode cylindrical fitting in such a conventional sodium-sulfur battery. The anode cylindrical metal fitting 3 includes a cylindrical portion 3a and a flange portion 3b projecting from the lower end of the cylindrical portion 3a toward the inside of the cylindrical portion 3a. The insulating ring 4 is inserted into the cylindrical portion 3a of the anode cylindrical metal fitting 3, and the upper surface of the flange portion 3b and the lower end surface of the insulating ring 4 are hot-pressure bonded through a bonding material 12 such as a metal brazing material. ing.
[0007]
Here, the insertion of the insulating ring 4 into the cylindrical portion 3a of the anode cylindrical metal fitting 3 is performed with a larger value C of the clearance 13 between the inner peripheral surface of the cylindrical portion 3a and the outer peripheral surface of the insulating ring 4. It is easy, and is particularly preferable when considering mass production and automation of assembly work. However, if the value C of the clearance 13 is too large, problems such as misalignment occur, and conventionally, the value C of the clearance 13 has been set to be about 1 mm.
[0008]
By the way, the sodium-sulfur battery has a temperature difference between when the battery is operated and when it is stopped. In a low temperature state when the battery is stopped, sodium polysulfide or sulfur is solidified, and the solid electrolyte tube 5 and the anode container 1 are mutually restrained. Will do. When the battery is cooled down, both the solid electrolyte tube 5 and the anode container 1 are thermally shrunk, but the heat shrinkage of the metal anode container 1 is large, and the shrinkage of the anode container 1 is suppressed to the solid electrolyte tube 5 having a small heat shrinkage. Therefore, a downward load is applied to the joint between the insulating ring 4 and the anode cylindrical fitting 3 that join the solid electrolyte tube 5 and the anode container 1 (in the direction of the arrow in FIG. 3).
[0009]
Therefore, conventionally, in order to prevent damage to the joint between the insulating ring 4 and the anode cylindrical fitting 3 due to this load, the inner circumferential surface contracts in the axial direction to a part of the circumferential surface of the anode container 1. Measures such as forming a constriction to provide a spring effect and reducing the load have been taken.
[0010]
[Problems to be solved by the invention]
However, even when the above measures are taken, cracks may occur if the joint end of the insulating ring 4 to the anode tubular fitting 3 is weak in strength. -It has become even more prominent as the size of sulfur batteries increases.
[0011]
The present invention has been made in view of such a situation, and an object of the present invention is to provide an insulating ring and an anode cylindrical shape against a load caused by a thermal contraction difference between the solid electrolyte tube and the anode container when the temperature of the battery is lowered. An object of the present invention is to provide a joint structure capable of improving the strength reliability of the joint portion with the metal fitting and preventing the joint portion from being damaged.
[0012]
[Means for Solving the Problems]
According to the present invention, an insulating ring is joined to the open end of the solid electrolyte tube, and a cylindrical portion coupled to the anode container and a flange portion protruding from the lower end of the cylindrical portion toward the inside of the cylindrical portion are connected to the insulating ring. A joining structure of an anode cylindrical fitting and an insulating ring of a sodium-sulfur battery, wherein the anode cylindrical fitting has a hot-pressure bonding through a bonding material so that the upper surface of the flange portion is joined to the lower end surface of the insulating ring. In this case, the value of the clearance between the inner peripheral surface of the cylindrical portion of the anode cylindrical metal fitting and the outer peripheral surface of the insulating ring is 0.15 mm or less, so that the bonding material soaks up to a position where the clearance is high. sodium and wherein the are - a structure for joining the insulating ring and the anode tubular fitting at sulfur battery, is provided.
[0013]
DETAILED DESCRIPTION OF THE INVENTION
In the joining structure of the insulating ring and the anode cylindrical metal fitting in the sodium-sulfur battery of the present invention, as shown in the cross-sectional view of the main part of FIG. 1, the inner peripheral surface of the cylindrical portion 3a of the anode cylindrical metal fitting 3 is insulated. The value C of the clearance 13 with the outer peripheral surface of the ring 4 is set to 0.15 mm or less, preferably 0.025 to 0.15 mm.
[0014]
Then, by setting the value C of the clearance 13 in this way, the joint structure of the present invention exhibits higher joint strength than the conventional joint structure in which the clearance value is set to about 1 mm. Although the reason for this is not clear, when the value C of the clearance 13 is set to be narrow so as to be 0.15 mm or less, as shown in FIG. 1, during the hot-pressure bonding between the anode cylindrical fitting 3 and the insulating ring 4, A joining material 12 such as a metal brazing material interposed between the upper surface of the flange portion 3b of the anode cylindrical metal fitting 3 and the lower end surface of the insulating ring 4 soaks up to a high position of the clearance 13 extending in the vertical direction, This is probably because the inner peripheral surface of the portion 3a and the outer peripheral surface of the insulating ring 4 are joined, and the joining area between the anode tubular fitting 3 and the insulating ring 4 increases.
[0015]
As described above, the present invention except that the value C of the clearance 13 between the inner peripheral surface of the cylindrical portion 3a of the anode cylindrical metal fitting 3 and the outer peripheral surface of the insulating ring 4 is set to be 0.15 mm or less. This joint structure is not different from the conventional joint structure described above. That is, as in the prior art, the insulating ring 4 is inserted into the cylindrical portion 3a of the anode cylindrical fitting 3, and the upper surface of the flange portion 13b of the anode cylindrical fitting 3 and the lower end surface of the insulating ring 4 are made of metal brazing material. Hot-pressure bonding is performed through a bonding material 12 such as the above.
[0016]
【Example】
EXAMPLES Hereinafter, although this invention is demonstrated further in detail based on an Example, this invention is not limited to these Examples.
[0017]
(Example)
Anode cylinders having various dimensions such that the value C of the clearance 13 between the inner peripheral surface of the cylindrical portion 3a and the outer peripheral surface of the insulating ring 4 shown in FIG. 1 is 0.025 to 0.3 mm as shown in Table 1. The metal fitting 3 and the insulating ring 4 were produced, and they were hot-pressure bonded to produce a test piece. As shown in FIG. 4, a load is applied from the upper part of the anode cylindrical fitting 3 to the test piece thus produced through the pushing jig 20, and the load is received by the receiving jig 21 at the lower part of the insulating ring 4. The fracture strength of the joint between the anode cylindrical metal fitting 3 and the insulating ring 4 was measured. The results are shown in Table 1 and FIG.
[0018]
[Table 1]
Figure 0003704241
[0019]
As shown in Table 1 and FIG. 5, the fracture strength decreases as the clearance value C increases, and it has been found that a high bonding strength can be obtained by setting the clearance value C to 0.15 mm or less.
[0020]
【The invention's effect】
As described above, according to the present invention, the strength reliability of the joint portion between the insulating ring and the anode cylindrical metal fitting can be improved, and by adopting this joint structure, the reliability of the sodium-sulfur battery can be improved. Can be increased.
[Brief description of the drawings]
FIG. 1 is a cross-sectional view of an essential part showing an embodiment of a bonding structure according to the present invention.
FIG. 2 is a cross-sectional view showing a general structure of a sodium-sulfur battery.
FIG. 3 is a cross-sectional view of a main part showing a conventional joining structure.
FIG. 4 is an explanatory diagram showing a method for measuring the fracture strength of a joint in an example.
FIG. 5 is a graph showing the results of Examples.
[Explanation of symbols]
DESCRIPTION OF SYMBOLS 1 ... Anode container, 2 ... Anode side terminal, 3 ... Anode cylindrical metal fitting, 4 ... Insulation ring, 5 ... Solid electrolyte tube, 6 ... Cartridge, 7 ... Small hole, 8 ... Cathode metal fitting, 9 ... Cathode lid, 10 ... Cathode side terminal, 11 ... partition wall tube, 12 ... bonding material, 13 ... clearance.

Claims (1)

固体電解質管の開口端に絶縁リングを接合し、当該絶縁リングに、陽極容器と結合した円筒部と当該円筒部下端から当該円筒部の内部方向に張り出したフランジ部とを有する陽極筒状金具を、前記フランジ部の上面が前記絶縁リングの下端面に接合されるように接合材を介して熱圧接合したナトリウム−硫黄電池の絶縁リングと陽極筒状金具との接合構造において、
前記陽極筒状金具の円筒部の内周面と、前記絶縁リングの外周面とのクリアランスの値が、０．１５ｍｍ以下であることにより、前記接合材が前記クリアランスの高い位置まで染み上がっていることを特徴とするナトリウム−硫黄電池における絶縁リングと陽極筒状金具との接合構造。An insulating ring is joined to the open end of the solid electrolyte tube, and an anode cylindrical fitting having a cylindrical portion coupled to the anode container and a flange portion projecting from the lower end of the cylindrical portion toward the inside of the cylindrical portion is attached to the insulating ring. In the joining structure between the insulating ring of the sodium-sulfur battery and the anode cylindrical fitting that are hot-pressure joined via a joining material so that the upper surface of the flange portion is joined to the lower end surface of the insulating ring,
When the value of the clearance between the inner peripheral surface of the cylindrical portion of the anode cylindrical metal fitting and the outer peripheral surface of the insulating ring is 0.15 mm or less, the bonding material soaks up to a position where the clearance is high. sodium and wherein the - junction structure between the insulating ring and the anode tubular fitting at sulfur battery.
JP26349798A 1998-09-17 1998-09-17 Joining structure of insulating ring and anode cylindrical fitting in sodium-sulfur battery Expired - Fee Related JP3704241B2 (en)

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