JPH0534782B2 - - Google Patents
Info
- Publication number
- JPH0534782B2 JPH0534782B2 JP59201701A JP20170184A JPH0534782B2 JP H0534782 B2 JPH0534782 B2 JP H0534782B2 JP 59201701 A JP59201701 A JP 59201701A JP 20170184 A JP20170184 A JP 20170184A JP H0534782 B2 JPH0534782 B2 JP H0534782B2
- Authority
- JP
- Japan
- Prior art keywords
- electrolyte
- phosphoric acid
- electrolyte layer
- electrode
- holder
- 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
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 claims description 62
- 239000003792 electrolyte Substances 0.000 claims description 52
- 229910000147 aluminium phosphate Inorganic materials 0.000 claims description 31
- 239000000446 fuel Substances 0.000 claims description 9
- 238000000034 method Methods 0.000 claims description 9
- -1 polytetrafluoroethylene Polymers 0.000 claims description 7
- 239000000758 substrate Substances 0.000 claims description 7
- 239000003054 catalyst Substances 0.000 claims description 6
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 6
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 6
- 239000000843 powder Substances 0.000 claims description 4
- 238000004519 manufacturing process Methods 0.000 claims description 3
- 239000002245 particle Substances 0.000 claims description 3
- 239000011159 matrix material Substances 0.000 claims description 2
- 150000003839 salts Chemical class 0.000 claims 1
- 238000010586 diagram Methods 0.000 description 4
- 239000000463 material Substances 0.000 description 3
- 238000010248 power generation Methods 0.000 description 3
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 3
- 229910010271 silicon carbide Inorganic materials 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 239000000470 constituent Substances 0.000 description 2
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 2
- 239000010452 phosphate Substances 0.000 description 2
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 239000011248 coating agent Substances 0.000 description 1
- 238000000576 coating method Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 230000008034 disappearance Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 239000011810 insulating material Substances 0.000 description 1
- 239000011244 liquid electrolyte Substances 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 239000012495 reaction gas Substances 0.000 description 1
- 230000000717 retained effect Effects 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 229910000166 zirconium phosphate Inorganic materials 0.000 description 1
- LEHFSLREWWMLPU-UHFFFAOYSA-B zirconium(4+);tetraphosphate Chemical compound [Zr+4].[Zr+4].[Zr+4].[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O.[O-]P([O-])([O-])=O LEHFSLREWWMLPU-UHFFFAOYSA-B 0.000 description 1
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
- H01M8/08—Fuel cells with aqueous electrolytes
-
- 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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04276—Arrangements for managing the electrolyte stream, e.g. heat exchange
- H01M8/04283—Supply means of electrolyte to or in matrix-fuel cells
-
- 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)
Description
【発明の詳細な説明】
〔発明の利用分野〕
本発明は電解質の補給を容易にした構造を有す
る燃料電池の製造方法に関する。DETAILED DESCRIPTION OF THE INVENTION [Field of Application of the Invention] The present invention relates to a method for manufacturing a fuel cell having a structure that facilitates replenishment of electrolyte.
液状の電解質を使用する燃料電池では、発電に
伴ない電解質が電池から飛散消失することが知ら
れている。例えば、リン酸を電解質とするリン酸
型燃料電池では、空気極における水の生成に伴な
つてリン酸が飛散するとされている。このため、
電池を長時間運転するとリン酸が不足して内部抵
抗が上昇し、電池性能が低下する。この内部抵抗
の上昇は次のように説明される。すなわち、リン
酸が不足して来ると、リン酸が保持されている電
解質層中に空隙が現われ、水素イオンの移動が阻
害される。このため、リン酸を電解質層へ補給す
る方法が種々提案されている。それらは２つに大
別される。１つは、電池の組立前に電極に予めリ
ン酸を電極に貯蔵（リザーブ）しておき、徐々に
リン酸を電解質層へ移動させる方法である（例え
ば、米国特許4115627号明細書参照）。他の１つ
は、電極の両端に接するセパレータにリン酸の
“ため”（リザーバ）を設け、これに電池外部から
通じる補給孔とリザーバから電解質層へ通じる補
給孔を設けてリン酸を補給する方法である（例え
ば特開昭54−154047号公報参照）。前者の方法で
は、反応ガスが拡散する電極の基板の細孔内にリ
ン酸がリザーブされるため、リザーブ量には限度
が有る。また、後者の方法では、電池を多数積層
した場合に補給孔の連結が困難である。
In fuel cells that use a liquid electrolyte, it is known that the electrolyte scatters and disappears from the cell as power is generated. For example, in a phosphoric acid fuel cell that uses phosphoric acid as an electrolyte, phosphoric acid is said to scatter as water is produced at the air electrode. For this reason,
When a battery is operated for a long time, phosphoric acid becomes insufficient, internal resistance increases, and battery performance deteriorates. This increase in internal resistance is explained as follows. That is, when phosphoric acid becomes insufficient, voids appear in the electrolyte layer in which phosphoric acid is retained, and the movement of hydrogen ions is inhibited. For this reason, various methods have been proposed for replenishing the electrolyte layer with phosphoric acid. They are broadly divided into two types. One is a method in which phosphoric acid is stored (reserved) in the electrode before battery assembly, and the phosphoric acid is gradually transferred to the electrolyte layer (see, for example, US Pat. No. 4,115,627). The other method is to provide a phosphoric acid "reservoir" in the separator that touches both ends of the electrode, and provide a replenishment hole leading from the outside of the battery and a replenishment hole leading from the reservoir to the electrolyte layer to replenish phosphoric acid. method (see, for example, Japanese Unexamined Patent Publication No. 154047/1983). In the former method, phosphoric acid is reserved in the pores of the electrode substrate through which the reaction gas diffuses, so there is a limit to the amount of phosphoric acid that can be reserved. Furthermore, in the latter method, it is difficult to connect the replenishment holes when a large number of batteries are stacked.
本発明の目的は、上記した従来技術の欠点を解
決し、電解質の補給が容易な燃料電池の製造方法
を提供するにある。
SUMMARY OF THE INVENTION An object of the present invention is to solve the above-described drawbacks of the prior art and to provide a method for manufacturing a fuel cell that allows easy replenishment of electrolyte.
本発明は、単位電池毎にリン酸のリザーバを設
け、かつリン酸が直接電解質層に移動するように
するため、電解質層の構成材料と同じ材料を用い
て電解質層とリザーバの間を連通させた点にあ
る。さらに具体的に述べれば、多孔質基板１４表
面に触媒層１３を設けてなる一方の電極の表面の
対向する２辺上の周囲に、電解質通路を有する電
解質層ホルダ８を載せ、該電解質層ホルダ８で挟
まれた前記触媒層１３の表面及び前記電解質層ホ
ルダ８内の電解質通路に電解質保持マトリツクス
材粒子をポリテトラフルオロエチレン又はリン酸
塩で結着させた粉末とリン酸とを混合してなるペ
ーストを充填して電解質層１０を形成し、該電解
質層１０の上に多孔質基板２表面に触媒層３を設
けた他方の電極を載せ、該他方の電極の対向する
２辺の両側の前記電解質層ホルダ８と対面する位
置に電解質貯蔵溝１２と該溝を前記電解質層ホル
ダ８内の電解質通路まで結ぶ貫通孔７とを有する
電極ホルダ６を配置し、前記一対の電極を外側か
ら加圧して前記ペーストの一部を前記電解質貯蔵
溝１２に到達するまで押し上げたのち該電解質貯
蔵溝１２にリン酸を貯蔵し、前記一対の電極の外
側からセパレータで締め付けるようにして燃料電
池を製造した点に本発明の特徴がある。リン酸型
燃料電池の電解質層は、一般にシリコンカーバイ
ドの微細粒子をポリテトラフルオロエチレンまた
はリン酸塩で結着させた粉末をリン酸と混合した
ペースト状の材料で形成される。したがつて、電
池の組立時に、一方の電極の周囲に少くとも一方
の面に電解質通路としてたとえば凹部を有する電
解質層ホルダを配し、前記ペーストを電極上に塗
布し、溝（リザーバ）及び貫通孔を有する電極ホ
ルダをリザーバが上となるように電解質層ホルダ
の上に配し、塗布されたペーストの上に電極を乗
せて押付けると、ペーストが電解質層ホルダの凹
部から電極ホルダの貫通孔を通つてリザーバに到
達し、リザーバから電解質層へのリン酸の補給路
が形成される。
In the present invention, a phosphoric acid reservoir is provided for each unit cell, and in order to allow phosphoric acid to move directly to the electrolyte layer, the electrolyte layer and the reservoir are communicated using the same material as the electrolyte layer. The point is that More specifically, an electrolyte layer holder 8 having electrolyte passages is placed around two opposing sides of the surface of one electrode, which is formed by providing a catalyst layer 13 on the surface of a porous substrate 14. 8 and the electrolyte passage in the electrolyte layer holder 8 are mixed with powder of electrolyte retention matrix material particles bound with polytetrafluoroethylene or phosphate and phosphoric acid. The electrolyte layer 10 is formed by filling a paste of An electrode holder 6 having an electrolyte storage groove 12 and a through hole 7 connecting the groove to an electrolyte passage in the electrolyte layer holder 8 is arranged at a position facing the electrolyte layer holder 8, and the pair of electrodes is applied from the outside. After pushing up a portion of the paste until it reached the electrolyte storage groove 12, phosphoric acid was stored in the electrolyte storage groove 12, and a separator was tightened from the outside of the pair of electrodes to produce a fuel cell. This is a feature of the present invention. The electrolyte layer of a phosphoric acid fuel cell is generally formed of a paste-like material made by mixing phosphoric acid with a powder of fine silicon carbide particles bound with polytetrafluoroethylene or phosphate. Therefore, when assembling the battery, an electrolyte layer holder is arranged around one electrode and has, for example, a recess as an electrolyte passage on at least one side, and the paste is applied onto the electrode, forming grooves (reservoirs) and through-holes. Place an electrode holder with a hole on top of the electrolyte layer holder with the reservoir facing up, place the electrode on top of the applied paste, and press it.The paste will flow from the recess of the electrolyte layer holder to the through hole of the electrode holder. A supply path for phosphoric acid from the reservoir to the electrolyte layer is formed.
電極ホルダは通常のカーボン板を加工すればよ
いが、リン酸を吸収する性質はできるだけないも
のがよい。リザーバ及び貫通孔の内壁はポリテト
ラフルオロエチレンコーテイングなどの不浸透処
理をしておくことが望ましい。リザーバの容積は
リン酸の消失量と電池の寿命の関係から決定され
る。貫通孔の数及び大きさはリン酸の消失速度か
ら決定される。電解質層の厚さはできるだけ薄い
方が電池の内部抵抗が小さくなつて望ましい。し
たがつて、電解質層ホルダの厚さは、0.1〜１mm、
望ましくは0.2〜0.5mmがよい。また、電解質層ホ
ルダの材料はポリテトラフルオロエチレン、シリ
コンカーバイトなど200℃前後でリン酸と実質的
に反応せず、かつ絶縁性の物質でなければならな
い。 The electrode holder may be made of a normal carbon plate, but it is preferable to use one that has as little ability to absorb phosphoric acid as possible. It is desirable that the inner walls of the reservoir and the through hole be treated with impermeability treatment such as polytetrafluoroethylene coating. The volume of the reservoir is determined from the relationship between the amount of phosphoric acid lost and the battery life. The number and size of through holes are determined by the rate of disappearance of phosphoric acid. It is desirable that the thickness of the electrolyte layer be as thin as possible because this will reduce the internal resistance of the battery. Therefore, the thickness of the electrolyte layer holder is 0.1 to 1 mm,
The thickness is preferably 0.2 to 0.5 mm. Furthermore, the material of the electrolyte layer holder must be an insulating material that does not substantially react with phosphoric acid at around 200° C., such as polytetrafluoroethylene or silicon carbide.
以下実施例によつて本発明をさらに詳しく説明
する。本発明の最も典型的な実施例を第１図に示
す。多孔質炭素基板１４の上に接触層１３を設け
た電極の上に、厚さ0.5mmのポリテトラフルオロ
エチレン板製電解質層ホルダ８を置き、電解質層
１０の部分にシリコンカーバイドをリン酸ジルコ
ニウムで結着させた微粉とリン酸を混合して調整
したペーストを塗り上から電極を乗せ、さらに電
極ホルダ６を乗せ、所定の圧力で押し付けた。リ
ザーバ１２へ溢れ出たペーストを除き、所定のリ
ン酸をリザーバ１２へ貯蔵し、上からセパレータ
１でしめ付け、電池を構成した。この電池に燃料
流路４から水素ガス、空気流路９から空気ガスを
供給して約200℃で連続発電した。なお、符号２
は基板、３は触媒層、１５はセパレータ、５はリ
ン酸を示している。その結果を第４図にとして
示す。またリザーバ１２、貫通孔７、凹部１１を
設けない以外は実施例と同じ電池を用いて連続発
電した結果をとして第４図に示す。本実施例に
より、電池の寿命が延びることが確認された。
The present invention will be explained in more detail below with reference to Examples. The most typical embodiment of the invention is shown in FIG. An electrolyte layer holder 8 made of a polytetrafluoroethylene plate with a thickness of 0.5 mm is placed on an electrode having a contact layer 13 provided on a porous carbon substrate 14, and silicon carbide is coated with zirconium phosphate on the electrolyte layer 10. A paste prepared by mixing the bound fine powder and phosphoric acid was applied, and an electrode was placed on top, and then an electrode holder 6 was placed on it and pressed with a predetermined pressure. After removing the paste that overflowed into the reservoir 12, a predetermined amount of phosphoric acid was stored in the reservoir 12, and a separator 1 was placed on top to form a battery. This battery was supplied with hydrogen gas from the fuel channel 4 and air gas from the air channel 9 to continuously generate electricity at about 200°C. In addition, code 2
1 is a substrate, 3 is a catalyst layer, 15 is a separator, and 5 is phosphoric acid. The results are shown in FIG. FIG. 4 shows the results of continuous power generation using the same battery as in the example except that the reservoir 12, through hole 7, and recess 11 were not provided. It was confirmed that this example extended the life of the battery.
以上、本発明の燃料電池は電解質の補給が容易
な構造となつているので、連続発電に適する。
As described above, since the fuel cell of the present invention has a structure that allows easy replenishment of electrolyte, it is suitable for continuous power generation.
第１図は本発明の典型的な実施例を示す電池の
構成図、第２図は本発明の構成要素である電解質
層ホルダの構成図、第３図は本発明の構成要素で
ある電極ホルダの構成図、第４図は本発明に基づ
いて構成した電池及び比較例による電池の連続発
電実験結果を示す特性図である。
１，１５……セパレータ、２，１４……基板、
３，１３……触媒層、５……リン酸、６……電極
ホルダ、７……貫通孔、８……電解質層ホルダ、
１０……電解質層、１１……凹部。
Fig. 1 is a block diagram of a battery showing a typical embodiment of the present invention, Fig. 2 is a block diagram of an electrolyte layer holder which is a constituent element of the present invention, and Fig. 3 is a block diagram of an electrode holder which is a constituent element of the present invention. FIG. 4 is a characteristic diagram showing the results of a continuous power generation experiment of a battery constructed based on the present invention and a battery according to a comparative example. 1, 15... Separator, 2, 14... Substrate,
3, 13... Catalyst layer, 5... Phosphoric acid, 6... Electrode holder, 7... Through hole, 8... Electrolyte layer holder,
10... Electrolyte layer, 11... Recessed part.
Claims (1)
る一方の電極の表面の対向する２辺上の周囲に、
電解質通路を有する電解質層ホルダ８を載せ、該
電解質層ホルダ８で挟まれた前記触媒層１３の表
面及び前記電解質層ホルダ８内の電解質通路に電
解質保持マトリツクス材粒子をポリテトラフルオ
ロエチレン又はリン酸塩で結着させた粉末とリン
酸とを混合してなるペーストを充填して電解質層
１０を形成し、該電解質層１０の上に多孔質基板
２表面に触媒層３を設けた他方の電極を載せ、該
他方の電極の対向する２辺の両側の前記電解質層
ホルダ８と対面する位置に電解質貯蔵溝１２と該
溝を前記電解質層ホルダ８内の電解質通路まで結
ぶ貫通孔７とを有する電極ホルダ６を配置し、前
記一対の電極を外側から加圧して前記ペーストの
一部を前記電解質貯蔵溝１２に到達するまで押し
上げたのち該電解質貯蔵溝１２にリン酸を貯蔵
し、前記一対の電極の外側からセパレータで締め
付けることを特徴とする燃料電池の製造方法。1 Around the two opposing sides of the surface of one electrode formed by providing the catalyst layer 13 on the surface of the porous substrate 14,
An electrolyte layer holder 8 having electrolyte passages is placed on the surface of the catalyst layer 13 sandwiched between the electrolyte layer holders 8 and the electrolyte passages in the electrolyte layer holder 8 with electrolyte retaining matrix material particles of polytetrafluoroethylene or phosphoric acid. The other electrode is filled with a paste made by mixing powder bound with salt and phosphoric acid to form an electrolyte layer 10, and a catalyst layer 3 is provided on the surface of a porous substrate 2 on the electrolyte layer 10. and has an electrolyte storage groove 12 at a position facing the electrolyte layer holder 8 on both opposing sides of the other electrode, and a through hole 7 connecting the groove to the electrolyte passage in the electrolyte layer holder 8. After placing the electrode holder 6 and pressurizing the pair of electrodes from the outside to push up a portion of the paste until it reaches the electrolyte storage groove 12, phosphoric acid is stored in the electrolyte storage groove 12. A method for manufacturing a fuel cell characterized by tightening an electrode with a separator from the outside.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59201701A JPS6180760A (en) | 1984-09-28 | 1984-09-28 | Fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59201701A JPS6180760A (en) | 1984-09-28 | 1984-09-28 | Fuel cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS6180760A JPS6180760A (en) | 1986-04-24 |
| JPH0534782B2 true JPH0534782B2 (en) | 1993-05-24 |
Family
ID=16445482
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP59201701A Granted JPS6180760A (en) | 1984-09-28 | 1984-09-28 | Fuel cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS6180760A (en) |
Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5848366A (en) * | 1981-09-17 | 1983-03-22 | Hitachi Ltd | Fuel cell |
| JPS58166652A (en) * | 1982-03-27 | 1983-10-01 | Hitachi Ltd | Electrolyte supplier of fuel cell |
-
1984
- 1984-09-28 JP JP59201701A patent/JPS6180760A/en active Granted
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPS5848366A (en) * | 1981-09-17 | 1983-03-22 | Hitachi Ltd | Fuel cell |
| JPS58166652A (en) * | 1982-03-27 | 1983-10-01 | Hitachi Ltd | Electrolyte supplier of fuel cell |
Also Published As
| Publication number | Publication date |
|---|---|
| JPS6180760A (en) | 1986-04-24 |
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Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| LAPS | Cancellation because of no payment of annual fees |