JP3229160B2 - Conductive bonding agent - Google Patents
Conductive bonding agentInfo
- Publication number
- JP3229160B2 JP3229160B2 JP08244095A JP8244095A JP3229160B2 JP 3229160 B2 JP3229160 B2 JP 3229160B2 JP 08244095 A JP08244095 A JP 08244095A JP 8244095 A JP8244095 A JP 8244095A JP 3229160 B2 JP3229160 B2 JP 3229160B2
- Authority
- JP
- Japan
- Prior art keywords
- bonding agent
- conductive bonding
- oxide
- electrode
- interconnector
- 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 - Lifetime
Links
- 239000007767 bonding agent Substances 0.000 title claims description 22
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 claims description 20
- 229910000480 nickel oxide Inorganic materials 0.000 claims description 11
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 claims description 11
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 10
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 10
- 239000000446 fuel Substances 0.000 claims description 9
- 239000000203 mixture Substances 0.000 claims description 5
- 238000005868 electrolysis reaction Methods 0.000 claims description 3
- 239000007784 solid electrolyte Substances 0.000 claims description 3
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 2
- 239000001257 hydrogen Substances 0.000 claims description 2
- 229910052739 hydrogen Inorganic materials 0.000 claims description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 6
- 238000010248 power generation Methods 0.000 description 6
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 4
- 229910052709 silver Inorganic materials 0.000 description 4
- 239000004332 silver Substances 0.000 description 4
- 229910001233 yttria-stabilized zirconia Inorganic materials 0.000 description 4
- OAYXUHPQHDHDDZ-UHFFFAOYSA-N 2-(2-butoxyethoxy)ethanol Chemical compound CCCCOCCOCCO OAYXUHPQHDHDDZ-UHFFFAOYSA-N 0.000 description 3
- 229910010413 TiO 2 Inorganic materials 0.000 description 3
- XEEYBQQBJWHFJM-UHFFFAOYSA-N iron Substances [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 229910052697 platinum Inorganic materials 0.000 description 3
- 239000007787 solid Substances 0.000 description 3
- LRHPLDYGYMQRHN-UHFFFAOYSA-N N-Butanol Chemical compound CCCCO LRHPLDYGYMQRHN-UHFFFAOYSA-N 0.000 description 2
- 239000000853 adhesive Substances 0.000 description 2
- 230000001070 adhesive effect Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 239000003960 organic solvent Substances 0.000 description 2
- 239000001293 FEMA 3089 Substances 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 239000007772 electrode material Substances 0.000 description 1
- 230000013011 mating Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 239000012528 membrane Substances 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 239000002994 raw material Substances 0.000 description 1
- 238000007650 screen-printing Methods 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052719 titanium Inorganic materials 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
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Landscapes
- Fuel Cell (AREA)
- Adhesives Or Adhesive Processes (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
- Conductive Materials (AREA)
Description
【０００１】[0001]
【産業上の利用分野】本発明は、固体電解質燃料電池あ
るいは水蒸気電解セルの電極と他の構成部材を電気的に
接合する場合に用いられる導電性接合剤に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a conductive bonding agent used for electrically connecting electrodes of a solid electrolyte fuel cell or a steam electrolysis cell to other components.
【０００２】[0002]
【従来の技術】周知の如く、固体電解質燃料電池（ＳＯ
ＦＣ）の一般構成としては、図２に示すものが知られて
いる。2. Description of the Related Art As is well known, a solid oxide fuel cell (SO
FIG. 2 shows a general configuration of the FC).
【０００３】図中の符番１は、イットリア安定化ジルコ
ニア２の両面に電極３ａ，３ｂが形成された発電膜であ
る。この発電膜１の上側には電極接続用波板４ａ，イン
タコネクタ５ａが形成され、下側には電極接続用波板４
ｂ，インタコネクタ５ｂが形成されている。Reference numeral 1 in the figure denotes a power generation film in which electrodes 3a and 3b are formed on both surfaces of yttria-stabilized zirconia 2. An electrode connecting corrugated sheet 4a and an interconnector 5a are formed on the upper side of the power generation film 1, and an electrode connecting corrugated sheet 4a is formed on the lower side.
b, an interconnector 5b is formed.
【０００４】こうした構成のＳＯＦＣにおいて、前記イ
ンタコネクタ５ａと電気接続用波板４ａとの間、電気接
続用波板４ａと電極３ａとの間、電極３ｂと電気接続用
波板４ｂとの間、電気接続用波板４ｂとインタコネクタ
５ｂとの間には、一般に導電性接合剤が用いられてい
る。[0004] In the SOFC having such a configuration, between the interconnector 5a and the corrugated plate 4a for electric connection, between the corrugated plate 4a for electric connection and the electrode 3a, between the electrode 3b and the corrugated plate 4b for electric connection, Generally, a conductive bonding agent is used between the electric connection corrugated plate 4b and the interconnector 5b.
【０００５】[0005]
【発明が解決しようとする課題】ところで、低温で下部
部材間を電気的に接合する場合は、前記導電性接合剤と
して銀ペースト，白金ペーストが知られている。ここ
で、銀ペーストは銀の電気抵抗が低く、導電性接着剤と
して一般的に使用されている。しかし、銀の融点は約９
６０℃であり、上記ＳＯＦＣのように１０００℃で充電
するものには使用できない。また、白金ペーストの場合
は１０００℃でも使用可能であるが、金属であるため熱
膨脹率が大きく、かつコスト高になるという問題点があ
る。When electrically connecting the lower members at a low temperature, silver paste and platinum paste are known as the conductive bonding agent. Here, silver paste has low electric resistance of silver and is generally used as a conductive adhesive. However, the melting point of silver is about 9
It is 60 ° C, and cannot be used for those charged at 1000 ° C, such as the SOFC. In the case of a platinum paste, it can be used even at 1000 ° C., but there is a problem in that since it is a metal, the coefficient of thermal expansion is large and the cost is high.
【０００６】本発明はこうした事情を考慮してなされた
もので、接合する電極と酸化ニッケル，酸化鉄，酸化チ
タンの混合物材料とすることにより、熱膨脹率の不一致
による剥離を極力抑えることができるとともに、接合力
を強くし、更にコスト低減を図ることができる導電性接
合剤を提供することを目的とする。The present invention has been made in view of such circumstances, and by using a mixture of nickel oxide, iron oxide, and titanium oxide as the electrode to be joined, peeling due to mismatch in thermal expansion coefficient can be suppressed as much as possible. It is an object of the present invention to provide a conductive bonding agent that can increase the bonding force and reduce the cost.
【０００７】[0007]
【課題を解決するための手段】本発明は、固体電解質燃
料電池あるいは水蒸気電解セルの水素電極とインタコネ
クタを電気的に接合する際に用いられる導電性接合剤に
おいて、酸化ニッケル，酸化鉄及び酸化チタンを含むこ
とを特徴とする導電性接合剤である。SUMMARY OF THE INVENTION The present invention relates to a conductive bonding agent used for electrically connecting a hydrogen electrode of a solid electrolyte fuel cell or a steam electrolysis cell to an interconnector. A conductive bonding agent containing titanium.
【０００８】本発明においては、前記酸化ニッケル，酸
化鉄及び酸化チタンの組成配合は、酸化ニッケル７０〜
９２％、酸化鉄３〜１０％、酸化チタン５〜２０％であ
ることが好ましい。In the present invention, the composition of the nickel oxide, the iron oxide and the titanium oxide is such that the nickel oxide is 70 to 70%.
Preferably, it is 92%, iron oxide 3 to 10%, and titanium oxide 5 to 20%.
【０００９】[0009]
【作用】本発明においては、接合する相手と同質の原料
である酸化ニッケルに酸化鉄及び酸化チタンを混合する
ことにより、接合強度を向上させることができると同時
に、熱膨脹率の低下により熱膨張の不一致による剥離を
極力防止することができ、良好な導電性接合剤を提供で
きるとともに、従来使用されていた白金に比べ大幅なコ
ストの低減が可能となる。In the present invention, by mixing iron oxide and titanium oxide with nickel oxide, which is a raw material of the same quality as the mating partner, the bonding strength can be improved, and at the same time, the thermal expansion coefficient is reduced due to a decrease in the thermal expansion coefficient. Separation due to mismatch can be prevented as much as possible, and a good conductive bonding agent can be provided. Further, the cost can be significantly reduced as compared with platinum conventionally used.
【００１０】[0010]
【実施例】以下、本発明の実施例について図面を参照し
て説明する。Embodiments of the present invention will be described below with reference to the drawings.
【００１１】（実施例１）図１を参照する。図中の符番
11は、イットリア安定化ジルコニア12の両面に酸化ニッ
ケルとＹＳＺの混合物の燃料側電極13ａ，酸素側電極13
ｂを形成した発電膜である。この発電膜11上には、導電
性接合剤14を介して電極接続用波板15が形成されてい
る。なお、ＳＯＦＣ全体の構成は、既述した図２に示す
ような構成となる。(Embodiment 1) Referring to FIG. Mark number in figure
Numeral 11 denotes a fuel-side electrode 13a and an oxygen-side electrode 13 of a mixture of nickel oxide and YSZ on both surfaces of yttria-stabilized zirconia 12.
This is a power generation film formed with b. An electrode connection corrugated plate 15 is formed on the power generation film 11 with a conductive bonding agent 14 interposed therebetween. Note that the overall configuration of the SOFC is as shown in FIG. 2 described above.
【００１２】前記導電性接合剤14は、次のようにして作
られる。即ち、燃料電池の燃料電極材料の酸化ニッケル
と酸化鉄，酸化チタンをそれぞれ酸化ニッケル７０〜９
２％、酸化鉄３〜１０％、酸化チタン５〜２０％で混合
し、有機溶媒としてブチルカルビトールを加え、ペース
ト状として導電性接合剤14を作る。なお、ブチルカルビ
トールの代りとしては粉体の分散性を向上させる他の溶
媒としてテレピン油，ブタノール等を使用してもよい。The conductive bonding agent 14 is made as follows. That is, nickel oxide, iron oxide, and titanium oxide as fuel electrode materials of the fuel cell are each converted to nickel oxide 70 to 9
2%, 3 to 10% of iron oxide and 5 to 20% of titanium oxide are mixed, butyl carbitol is added as an organic solvent, and the conductive bonding agent 14 is prepared in the form of a paste. Instead of butyl carbitol, turpentine oil, butanol or the like may be used as another solvent for improving the dispersibility of the powder.
【００１３】前記導電性接合剤14は、接着剤として前記
燃料側電極13ａと電極接続用波板15を接着した後、導電
性接合剤14による接合を行う。The conductive bonding agent 14 is bonded by using the conductive bonding agent 14 after the fuel-side electrode 13a and the electrode connecting corrugated plate 15 are bonded as an adhesive.
【００１４】上記実施例１においては、発電膜11の構成
である燃料側電極13ａと電極接続用波板15を接続する導
電性接合剤14が燃料側電極13ａと電気的抵抗の低い接着
を可能とする。導電性接合剤14は、酸化ニッケル，酸化
鉄，酸化チタンの混合物をブチルカルビトール等のビヒ
クル（有機溶媒）を用いてペースト状としたものを、ス
クリーンにあいた穴から印刷するスクリーンプリントの
方法によりインタコネクタ平板上に１００〜２００μｍ
の厚さに均一に塗布し、接続用波板を乗せた後、空気中
で熱処理を行う。In the first embodiment, the conductive bonding agent 14 for connecting the fuel-side electrode 13a and the corrugated plate 15 for electrode connection, which constitute the power generation film 11, enables the fuel-side electrode 13a to be bonded to the fuel-side electrode 13a with low electrical resistance. And The conductive bonding agent 14 is prepared by a screen printing method in which a mixture of nickel oxide, iron oxide, and titanium oxide is made into a paste using a vehicle (organic solvent) such as butyl carbitol, and is printed through a hole formed in the screen. 100-200μm on interconnector flat plate
And heat-treated in the air after placing a connecting corrugated plate.
【００１５】（実施例２）２０ｍｍ角のインタコネクタ
材料と電気接続用の波板のテストピース部品をＴｉＯ2
−Ｆｅ2 Ｏ3 −ＮｉＯ系接続材料を用いて接続し、接着
性，導電性について検討した。良好な接着性及び導電性
を示す範囲は、図３に示す通りであった。(Example 2) A test piece part of a 20 mm square interconnector material and a corrugated sheet for electrical connection was made of TiO 2
Connect with -Fe 2 O 3 -NiO-based connecting material was studied adhesion, conductivity about. The range showing good adhesion and conductivity was as shown in FIG.
【００１６】図３において、各頂点は成分１００％のポ
イントを示す。ＴｉＯ2 は接着性を向上し、ＮｉＯは導
電性を示し、Ｆｅ2 Ｏ3 は接着性を補助的に向上すると
同時に導電性も保有する。以上より、導電性の接合材料
として好ましい範囲は、図３の斜線部分Ｘに示す狭い範
囲である。In FIG. 3, each vertex indicates a point of 100% of the component. TiO 2 improves the adhesiveness, NiO shows conductivity, and Fe 2 O 3 supplementarily improves the adhesiveness and also retains conductivity. As described above, a preferable range for the conductive bonding material is a narrow range indicated by a hatched portion X in FIG.
【００１７】[0017]
【発明の効果】以上詳述したようにこの発明によれば、
熱膨脹率の不一致による剥離を極力抑えることができる
とともに、接合力を強くし、更にコスト低減を図ること
ができる導電性接合剤を提供できる。As described in detail above, according to the present invention,
It is possible to provide a conductive bonding agent that can minimize peeling due to mismatch in thermal expansion coefficient, increase bonding strength, and further reduce cost.
【図１】本発明の実施例１に係る導電性接合剤を用いた
固体電解質燃料電池の要部の説明図。FIG. 1 is an explanatory diagram of a main part of a solid oxide fuel cell using a conductive bonding agent according to a first embodiment of the present invention.
【図２】固体電解質燃料電池を展開した概略斜視図。FIG. 2 is a schematic perspective view in which a solid oxide fuel cell is developed.
【図３】本発明に係る導電性接合剤の適正範囲を示すＮ
ｉＯ，Ｆｅ2 Ｏ3 ，ＴｉＯ2 三相成分図。FIG. 3 shows an appropriate range of the conductive bonding agent according to the present invention.
FIG. 3 is a three-phase component diagram of iO, Fe 2 O 3 , and TiO 2 .
11…発電膜、 12…イットリア安定化ジルコニア、
12ａ…燃料側電極、12ｂ…酸素側電極、14…導電性接合
剤、 15…電極接続用波板。11 ... power generation membrane, 12 ... yttria stabilized zirconia,
12a: fuel side electrode, 12b: oxygen side electrode, 14: conductive bonding agent, 15: corrugated plate for electrode connection.
───────────────────────────────────────────────────── フロントページの続き (51)Int.Cl.7 識別記号 ＦＩ Ｈ０１Ｍ 8/12 Ｈ０１Ｍ 8/12 (58)調査した分野(Int.Cl.7，ＤＢ名) H01M 8/02 C25B 9/04 H01M 8/12 H01B 1/20 ──────────────────────────────────────────────────の Continuation of the front page (51) Int.Cl. 7 identification code FI H01M 8/12 H01M 8/12 (58) Investigated field (Int.Cl. 7 , DB name) H01M 8/02 C25B 9/04 H01M 8/12 H01B 1/20
Claims (2)
セルの水素電極とインタコネクタを電気的に接合する際
に用いられる導電性接合剤において、酸化ニッケル，酸
化鉄及び酸化チタンを含むことを特徴とする導電性接合
剤。1. A conductive bonding agent used for electrically connecting a hydrogen electrode of a solid electrolyte fuel cell or a steam electrolysis cell to an interconnector, comprising nickel oxide, iron oxide and titanium oxide. Conductive bonding agent.
ンの組成配合が、それぞれ酸化ニッケル７０〜９２％、
酸化鉄３〜１０％、酸化チタン５〜２０％であることを
特徴とする請求項１記載の導電性接合剤。2. The composition of nickel oxide, iron oxide and titanium oxide is 70-92% nickel oxide,
The conductive bonding agent according to claim 1, wherein the content is 3 to 10% of iron oxide and 5 to 20% of titanium oxide.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP08244095A JP3229160B2 (en) | 1995-04-07 | 1995-04-07 | Conductive bonding agent |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP08244095A JP3229160B2 (en) | 1995-04-07 | 1995-04-07 | Conductive bonding agent |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPH08287930A JPH08287930A (en) | 1996-11-01 |
| JP3229160B2 true JP3229160B2 (en) | 2001-11-12 |
Family
ID=13774610
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP08244095A Expired - Lifetime JP3229160B2 (en) | 1995-04-07 | 1995-04-07 | Conductive bonding agent |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JP3229160B2 (en) |
Families Citing this family (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP5075183B2 (en) * | 2009-02-04 | 2012-11-14 | 日本碍子株式会社 | Electrochemical equipment |
| JP5330849B2 (en) * | 2009-02-12 | 2013-10-30 | 三菱重工業株式会社 | Conductive bonding material and solid oxide fuel cell having the same |
| CN103460473B (en) | 2011-03-30 | 2014-10-15 | 株式会社村田制作所 | Fuel cell |
| WO2012132893A1 (en) * | 2011-03-30 | 2012-10-04 | 株式会社村田製作所 | Fuel cell |
-
1995
- 1995-04-07 JP JP08244095A patent/JP3229160B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| JPH08287930A (en) | 1996-11-01 |
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