JPS58128667A - Fuel cell - Google Patents
Fuel cellInfo
- Publication number
- JPS58128667A JPS58128667A JP57009006A JP900682A JPS58128667A JP S58128667 A JPS58128667 A JP S58128667A JP 57009006 A JP57009006 A JP 57009006A JP 900682 A JP900682 A JP 900682A JP S58128667 A JPS58128667 A JP S58128667A
- Authority
- JP
- Japan
- Prior art keywords
- electrode
- gas diffusion
- fuel cell
- seal
- electrolyte
- 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.)
- Pending
Links
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
-
- 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
- Life Sciences & Earth Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Fuel Cell (AREA)
Abstract
Description
【発明の詳細な説明】
本発明は多孔性ガス拡散電極を用いる燃料電池に係り、
特に多孔性ガス拡散電極の端部からのガスもれを防止す
るに好適な端部シールを備えたリン酸型燃料電池に関す
る。DETAILED DESCRIPTION OF THE INVENTION The present invention relates to a fuel cell using a porous gas diffusion electrode,
In particular, the present invention relates to a phosphoric acid fuel cell equipped with an end seal suitable for preventing gas leakage from the end of a porous gas diffusion electrode.
天然ガスやメタンなどの改質ガスあるいは純水素を燃料
とし、空気や純酸素を酸化剤として用いる種類の燃料電
池では、多孔性のガス拡散電極が用いられる。多孔性ガ
ス拡散電極では、その端部から燃料や酸化剤が漏洩しな
いように１端部を気密にしなければならない。従来、こ
の端部シール法としては％升えはリン酸を電解質として
用いる燃料電池工は、ウェットシールと呼ばれる方法が
採用されてい友。すなわち、多孔性ガス拡散電極として
、炭素繊維からなるカーボンベーパト呼ばれるものの上
に触媒層を設けたものを用い、その端部にリン酸を保持
した物質、一般にシリコンカーバイド、ポリテトラフル
オロエチレン及びリン酸を混合した物質を塗り込むとい
う方法が用いられてい友。しかし、この方法ではリン酸
が液体であるために、長時間燃料電池を運転していると
、リン酸が蒸発し、そのためにシール性がなくなり。Porous gas diffusion electrodes are used in fuel cells of the type that use reformed gas such as natural gas or methane or pure hydrogen as a fuel and air or pure oxygen as an oxidizing agent. A porous gas diffusion electrode must be airtight at one end to prevent fuel or oxidant from leaking from the end. Conventionally, fuel cell engineers using phosphoric acid as an electrolyte have adopted a method called wet sealing for this end sealing method. That is, as a porous gas diffusion electrode, a catalyst layer is provided on carbon fiber made of carbon vapor, and a material holding phosphoric acid, generally silicon carbide, polytetrafluoroethylene, and phosphorus, is used at the end. A method of applying a substance mixed with acid is used. However, in this method, since the phosphoric acid is a liquid, if the fuel cell is operated for a long time, the phosphoric acid evaporates, resulting in loss of sealing performance.
ガスが透過するという大きな欠点があった。The major drawback was that gas permeated through it.
本発明の目的は従来技術の欠点１［り除き、長期間の運
転で本気密性を失なわない端部シールを有する燃料電池
を提供するにある。SUMMARY OF THE INVENTION The object of the present invention is to eliminate the drawbacks of the prior art and to provide a fuel cell having end seals that do not lose their airtightness even after long-term operation.
本発明は、多孔性ガス拡散電極の端部シールを気密性を
有する固体物質で構成するものである。According to the present invention, the end seal of a porous gas diffusion electrode is made of a solid material having airtightness.
気密性を有する固体物質としては、金属リン酸塩が好適
である。ジルコニウム、チタン、スズ。A metal phosphate is suitable as the airtight solid substance. Zirconium, titanium, tin.
アルミニウム、ケイ素、カルシウムなどの金属塩あるい
はこれらの酸化物はリン酸と反応して、金属リン酸塩を
作る。この金属リン酸塩は固体であり、これが多孔性ガ
ス拡散電極の周囲の孔中に形成されると、穴を密閉し、
ガスの漏洩を防止する。Metal salts such as aluminum, silicon, calcium, or their oxides react with phosphoric acid to form metal phosphates. This metal phosphate is a solid, and when it forms in the pores around the porous gas diffusion electrode, it seals the pores and
Prevent gas leakage.
本発明による多孔性ガス拡散電極は、炭素繊維からなる
カーボンベーパ、炭素粉末焼結体、あるいは耐酸性や耐
アルカリ性を有する金属粉末の焼結体などを基板とし、
必ｌ！に応じてこれらに触媒層を設けたものである。The porous gas diffusion electrode according to the present invention uses a carbon vapor made of carbon fiber, a sintered body of carbon powder, or a sintered body of metal powder having acid resistance and alkali resistance as a substrate,
Must! A catalyst layer is provided on these according to the requirements.
なお、金属リン酸塩はシリコンカーバイド、ジルコン、
カーボンなどのように電解質に対して耐食性を有する物
質を含んだ状態で形成されてもさしつかえない。In addition, metal phosphates include silicon carbide, zircon,
It may be formed in a state containing a substance that is resistant to corrosion against electrolytes, such as carbon.
以下、本発明の具体的な実施例を述べる。Hereinafter, specific examples of the present invention will be described.
実施例１ 多孔性ガス電極の基板として、気孔率８０％。Example 1 As a substrate for porous gas electrodes, porosity is 80%.
厚さ０．３５ｍの炭素線維製カーボンベーパを用いた。Carbon fiber carbon vapor having a thickness of 0.35 m was used.
基板の寸法は４０１角とし１周囲１帰幅を残して触媒層
を設けた。触媒は通常の方法によって。The dimensions of the substrate were 401 square meters, and the catalyst layer was provided with one width left over one circumference. Catalyst by the usual method.
炭素粉末に貴金属を付着させた本のである。触媒層の庫
さは０．０５ｍとした。この電極を空気中３１０Ｃで３
０分間焼成したのち、酸化ジルコニウムとリン酸の混合
物を周囲１ｃｗ１の幅で触媒を塗布していない部分の気
孔中ＫＮ！り込んだ６酸化ジルコニウムとリン酸の混合
量は酸化ジルコニウムムロ０ｇ、リン酸９５．６ｇ＆Ｃ
した。この混合物１６ｇを分取し、気孔を完全に密閉し
九。次圧電極を２００Ｃで１５時間加熱し、酸化ジルコ
ニウムとリン酸の反応を完了した。このときの反応は。This is a book with precious metals attached to carbon powder. The height of the catalyst layer was 0.05 m. This electrode was heated at 310C in air for 3
After firing for 0 minutes, a mixture of zirconium oxide and phosphoric acid was applied to the pores of the area where the catalyst was not coated with a width of 1 cw1. The mixed amount of zirconium hexoxide and phosphoric acid is 0 g of zirconium oxide, 95.6 g of phosphoric acid &C
did. Take 16 g of this mixture and completely seal the pores. The subpressure electrode was heated at 200 C for 15 hours to complete the reaction between zirconium oxide and phosphoric acid. What was your reaction at this time?
次式の通りでおる。It is as follows.
Ｚ ｒ Ｏ＊ ＋ ２Ｈｓ Ｐ Ｏｎ →Ｚ ’ （Ｈ
Ｐ ０４ ）１ ＋ ２Ｈｘ ０以上の手順で得た多孔
性ガス拡散陽極の状態を第１図に示す。１は多孔性ガス
拡散電極の基板として取シあげたカーボン繊維からなる
カーボンベーパ、 ２／ｒｉ炭素粉末に貴金属を付着さ
せ九触媒を塗布した触媒層、３は本発明による金属リン
酸塩をカーボンベーパの気孔中に存在させた基部シール
部である。第２図に第１図で示した基部シール部を拡大
した断面図を示す。Z r O* + 2Hs P On →Z' (H
P 04 )1 + 2Hx 0 The state of the porous gas diffusion anode obtained by the above procedure is shown in FIG. 1 is a carbon vapor made of carbon fiber used as a substrate for a porous gas diffusion electrode; 2 is a catalyst layer made by adhering a noble metal to RI carbon powder and coating a catalyst; 3 is a carbon vapor made of carbon fiber using a metal phosphate according to the present invention. This is a base seal located in the pores of the vapor. FIG. 2 shows an enlarged sectional view of the base seal portion shown in FIG. 1.
第１図に示した多孔性ガス電極を用い、第３図に示した
セル合繊み立てて、端部シール部の気密性を調べ九。第
３図において、４ｉｉガス不透過処理１ｋｌｌＩＡシた
黒鉛板を加工したセル枠であり、内部にガス室を形成す
る凹凸が設けられている。５は本発明による端部シール
を有する多孔性ガス拡散電極、６はフッ素ゴムからなる
ガスケット、７は電解質であるリン酸を保持したマトリ
ックス、８はセルを締付けるための押え板、９は締付は
ボルト、１０はナラ）、１１はセル内にガスを供給また
は排気するためのガス供給＃排出口でおる。第３図に示
したセルを恒温槽に入れ、温度ｔ−２００ＣＫＬ＆後、
ガス供給、排出口１１からセル内のガスを排気し、セ
ル内を真空状１１１１Ｋした。この状態で長時間放置し
たときのセル内のガス圧力を調べ、端部シール部の気密
性を評価し丸。第４図はセル内の圧力変化と経時時間を
示し友ものである。Using the porous gas electrode shown in Fig. 1, the cell composite shown in Fig. 3 was assembled, and the airtightness of the end seal was examined.9. In FIG. 3, the cell frame is made of a graphite plate that has been subjected to 4II gas impermeability treatment by 1kllIA, and is provided with unevenness to form a gas chamber inside. 5 is a porous gas diffusion electrode having an end seal according to the present invention, 6 is a gasket made of fluororubber, 7 is a matrix holding phosphoric acid as an electrolyte, 8 is a holding plate for tightening the cell, and 9 is a tightening plate. 10 is a bolt, 11 is a gas supply/exhaust port for supplying or exhausting gas into the cell. The cell shown in Figure 3 was placed in a constant temperature bath, and after the temperature was t-200CKL,
The gas inside the cell was exhausted from the gas supply and exhaust ports 11, and the inside of the cell was evacuated to 1111K. We checked the gas pressure inside the cell when it was left in this state for a long time, and evaluated the airtightness of the end seal. Figure 4 shows the change in pressure inside the cell and the elapsed time.
第４図において、記号人で示しｆｅ、−のが本発明によ
る多孔性ガス拡散電極を用い友ものでめシ、記号Ｂは従
来のウェットシールによるものである。In FIG. 4, the symbols fe and - are those using the porous gas diffusion electrode according to the present invention, and the symbols B are those using the conventional wet seal.
第４図から明らかなように５本発明によると、多孔性ガ
ス拡散電極の周辺が気密になる九めに、はとんどガスの
透過がないことが判る。As is clear from FIG. 4, according to the present invention, when the area around the porous gas diffusion electrode becomes airtight, there is almost no gas permeation.
実施例２ 実施例１と同様、多孔性ガス電極基板として。Example 2 As in Example 1, as a porous gas electrode substrate.
カーボンベーパを用い、周辺部にシリコンカーバイド、
ｍ化ジルコニウム、及びリン酸の混合物をｍ、６込んだ
。シリコンカーバイド、酸化ジルコニウム、リン酸の混
合割合は５：２：３とし、この混合物１２ｇを用いた。Using carbon vapor, silicon carbide on the periphery,
A mixture of zirconium mide and phosphoric acid was charged into the tank. The mixing ratio of silicon carbide, zirconium oxide, and phosphoric acid was 5:2:3, and 12 g of this mixture was used.
実施例１と同一の温度で加熱したのち、第３図に示した
セルを用いて、気密性を調べたところ、第４図、記号Ａ
で示したと同様な結果を得ることができた。After heating at the same temperature as in Example 1, the airtightness was examined using the cell shown in Figure 3.
We were able to obtain results similar to those shown in .
以上記した実施例の他に、硝酸ジルコニル、オキシ塩化
ジルコニウムなどのジルコニウム塩、スズ、チタン、ア
ルミニウム、カルシウム、ケイ素などの堪およびこれら
の酸化物を用いて実施例１゜２に示したと同様に気密性
を調べたところ、第４図に示したと、はぼ同じ結果を得
ることができた。In addition to the examples described above, zirconium salts such as zirconyl nitrate and zirconium oxychloride, metals such as tin, titanium, aluminum, calcium, and silicon, and oxides thereof were used in the same manner as shown in Example 1-2. When we investigated the airtightness, we were able to obtain almost the same results as shown in Figure 4.
以上述べたように本発明は多孔性ガス拡散電極の端部か
らのガス漏洩をなくシ、すぐれた性質を有するものであ
る。したがって、その工業的価値は極めて大である。As described above, the present invention eliminates gas leakage from the ends of the porous gas diffusion electrode and has excellent properties. Therefore, its industrial value is extremely large.
第１図は本発明による端部シールを設けた多孔性ガス拡
散電極の斜視図、第２図は多孔性ガス電極の端部シール
部の拡大断面図、第３図は本発明の一夾施例會示す燃料
電池の断面図、第４図は時間とセル内の気密性の関係を
調べ九結果を示す特性図である。
３・・・端部シール部、５・・・多孔性ガス拡散電極、
７某 ｔｍ
ａ手ｒｌｉ１（＃Ｌ）
第１頁の続き
０発 明 者 本地量大
日立市幸町３丁目１番１号株式
％式％
０出 願 人 日立化成工業株式会社
東京都新宿区西新宿２丁目１番
１号FIG. 1 is a perspective view of a porous gas diffusion electrode provided with an end seal according to the present invention, FIG. 2 is an enlarged cross-sectional view of the end seal portion of the porous gas electrode, and FIG. 3 is a perspective view of a porous gas diffusion electrode provided with an end seal according to the present invention. FIG. 4, which is a cross-sectional view of the fuel cell shown in the example, is a characteristic diagram showing the results of examining the relationship between time and airtightness within the cell. 3... End seal part, 5... Porous gas diffusion electrode,
7 certain tm a hand rli1 (#L) Continued from page 1 0 Inventor: Land amount 3-1-1 Saiwaimachi, Dahitachi City Stock% formula % 0 Applicant: Hitachi Chemical Co., Ltd. Nishi, Shinjuku-ku, Tokyo Shinjuku 2-1-1
Claims (1)
肩質保持オトリックスと、前記マトリックス内に配置さ
れた電解質及び前記電極端部のシールとを有するものに
おいて、前記シールが気密性を有する固体物質により構
成されていることを特徴とする燃料電池。 ２ ％許請求の＃ｌｉ囲第１項において、＊記気密性を
有する物質がジルコニウム、スズ、チタン、アルイニウ
ム、ケイ素、カルシウムの少なくとも１ｍｓ＋を含む金
属リン酸塩からなることを特徴とする燃料電池。 λ 特許請求の範囲第１項において、前記気密性を有す
る物質が、金属リン酸塩と電解質に対して耐食性を有す
る物質との混合物からなることを特徴とする燃料電池。 ４．４Ｉ許請求の範囲＃Ｉ１項において、前記電解質に
対して耐食性を有する物質が、シリコンカーバイド、ジ
ルコン及びカーボンの少なくとも１つからなることを特
徴とする燃料電池。[Claims] 1. A gas diffusion electrode comprising a pair of gas diffusion electrodes, an electrolyte holding ottrix disposed between the electrodes, an electrolyte disposed within the matrix, and a seal at the end of the electrode. . A fuel cell, wherein the seal is made of an airtight solid material. 2. A fuel cell according to item 1 of box #li of the claim, characterized in that the substance having airtightness is made of a metal phosphate containing at least 1ms+ of zirconium, tin, titanium, aluminum, silicon, and calcium. . λ The fuel cell according to claim 1, wherein the airtight substance is made of a mixture of a metal phosphate and a substance that is corrosion resistant to the electrolyte. 4.4I The fuel cell according to claim #I1, wherein the substance having corrosion resistance to the electrolyte is comprised of at least one of silicon carbide, zircon, and carbon.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP57009006A JPS58128667A (en) | 1982-01-25 | 1982-01-25 | Fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP57009006A JPS58128667A (en) | 1982-01-25 | 1982-01-25 | Fuel cell |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS58128667A true JPS58128667A (en) | 1983-08-01 |
Family
ID=11708564
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP57009006A Pending JPS58128667A (en) | 1982-01-25 | 1982-01-25 | Fuel cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS58128667A (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS63126169A (en) * | 1986-11-17 | 1988-05-30 | Toshiba Corp | Manufacture of end seal for phosphoric acid type fuel cell electrode |
| JPS63181266A (en) * | 1987-01-21 | 1988-07-26 | Mitsubishi Electric Corp | Gas sealing method for phosphoric acid type fuel cell |
| US5173373A (en) * | 1989-09-14 | 1992-12-22 | Yamaha Hatsudoki Kabushiki Kaisha | Gasket for fuel cell |
| CN114243039A (en) * | 2022-02-28 | 2022-03-25 | 浙江高成绿能科技有限公司 | High-temperature-resistant composite carrier, catalyst for fuel cell and preparation method thereof |
-
1982
- 1982-01-25 JP JP57009006A patent/JPS58128667A/en active Pending
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS63126169A (en) * | 1986-11-17 | 1988-05-30 | Toshiba Corp | Manufacture of end seal for phosphoric acid type fuel cell electrode |
| JPS63181266A (en) * | 1987-01-21 | 1988-07-26 | Mitsubishi Electric Corp | Gas sealing method for phosphoric acid type fuel cell |
| US5173373A (en) * | 1989-09-14 | 1992-12-22 | Yamaha Hatsudoki Kabushiki Kaisha | Gasket for fuel cell |
| US5407759A (en) * | 1989-09-14 | 1995-04-18 | Yamaha Hatsudoki Kabushiki Kaisha | Gasket for fuel cell |
| CN114243039A (en) * | 2022-02-28 | 2022-03-25 | 浙江高成绿能科技有限公司 | High-temperature-resistant composite carrier, catalyst for fuel cell and preparation method thereof |
| CN114243039B (en) * | 2022-02-28 | 2022-05-27 | 浙江高成绿能科技有限公司 | High-temperature-resistant composite carrier, catalyst for fuel cell and preparation method of catalyst |
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