JPS63277736A - Separator for phosphoric acid type fuel cell - Google Patents
Separator for phosphoric acid type fuel cellInfo
- Publication number
- JPS63277736A JPS63277736A JP62111467A JP11146787A JPS63277736A JP S63277736 A JPS63277736 A JP S63277736A JP 62111467 A JP62111467 A JP 62111467A JP 11146787 A JP11146787 A JP 11146787A JP S63277736 A JPS63277736 A JP S63277736A
- Authority
- JP
- Japan
- Prior art keywords
- separator
- phosphoric acid
- fuel cell
- amorphous alloy
- acid fuel
- 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
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 title claims abstract description 42
- 229910000147 aluminium phosphate Inorganic materials 0.000 title claims abstract description 21
- 239000000446 fuel Substances 0.000 title claims abstract description 20
- 229910000808 amorphous metal alloy Inorganic materials 0.000 claims abstract description 13
- 229910052710 silicon Inorganic materials 0.000 claims abstract description 6
- 239000012535 impurity Substances 0.000 claims abstract description 5
- 238000005260 corrosion Methods 0.000 abstract description 9
- 230000007797 corrosion Effects 0.000 abstract description 9
- 229910045601 alloy Inorganic materials 0.000 abstract description 5
- 239000000956 alloy Substances 0.000 abstract description 5
- 230000001105 regulatory effect Effects 0.000 abstract 1
- 125000004429 atom Chemical group 0.000 description 14
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 13
- 229910052799 carbon Inorganic materials 0.000 description 13
- 230000000694 effects Effects 0.000 description 6
- 230000007423 decrease Effects 0.000 description 4
- 239000000203 mixture Substances 0.000 description 4
- 230000001681 protective effect Effects 0.000 description 4
- 230000015572 biosynthetic process Effects 0.000 description 3
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 238000005096 rolling process Methods 0.000 description 3
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 2
- 229910019142 PO4 Inorganic materials 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 239000003054 catalyst Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 239000003792 electrolyte Substances 0.000 description 2
- 238000003754 machining Methods 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- XDTMQSROBMDMFD-UHFFFAOYSA-N Cyclohexane Chemical compound C1CCCCC1 XDTMQSROBMDMFD-UHFFFAOYSA-N 0.000 description 1
- 238000002441 X-ray diffraction Methods 0.000 description 1
- 229910052786 argon Inorganic materials 0.000 description 1
- 239000012300 argon atmosphere Substances 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 238000005336 cracking Methods 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 238000002844 melting Methods 0.000 description 1
- 230000008018 melting Effects 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 125000004430 oxygen atom Chemical group O* 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- RMAQACBXLXPBSY-UHFFFAOYSA-N silicic acid Chemical class O[Si](O)(O)O RMAQACBXLXPBSY-UHFFFAOYSA-N 0.000 description 1
- HBMJWWWQQXIZIP-UHFFFAOYSA-N silicon carbide Chemical compound [Si+]#[C-] HBMJWWWQQXIZIP-UHFFFAOYSA-N 0.000 description 1
- 229910010271 silicon carbide Inorganic materials 0.000 description 1
- 235000012239 silicon dioxide Nutrition 0.000 description 1
- 230000004580 weight loss Effects 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C45/00—Amorphous alloys
- C22C45/10—Amorphous alloys with molybdenum, tungsten, niobium, tantalum, titanium, or zirconium or Hf as the major constituent
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C45/00—Amorphous alloys
- C22C45/04—Amorphous alloys with nickel or cobalt as the major constituent
Abstract
Description
【発明の詳細な説明】
〔産業上の利用分野〕
この発明は、りん酸型燃料電池のセパレーターに関する
ものである。DETAILED DESCRIPTION OF THE INVENTION [Field of Industrial Application] This invention relates to a separator for phosphoric acid fuel cells.
一般に、りん酸型燃料電池を構成するセルは。 Generally, the cells that make up a phosphoric acid fuel cell are:
第１図に示される構造となっており、かかる構造のセル
が、例えば２００層程変種層されて組込まれてりん酸型
燃料電池を構成していた。The structure was as shown in FIG. 1, and a phosphoric acid fuel cell was constructed by incorporating, for example, about 200 different layers of cells having this structure.
第１図は、シん酸型燃料電池のセルの構造を示す概略図
であシ、１はセパレーター、２は負極、３は電極触媒、
４は電解質、５は正極を示す。FIG. 1 is a schematic diagram showing the structure of a silicic acid fuel cell, in which 1 is a separator, 2 is a negative electrode, 3 is an electrode catalyst,
4 represents an electrolyte, and 5 represents a positive electrode.
上記りん酸型燃料電池用セルにおけるセパレーター１の
材料として、次のような特性が求められている。The following characteristics are required for the material of the separator 1 in the above-mentioned phosphoric acid fuel cell.
（１） 高温濃縮りん酸に対する耐食性が高いこと。(1) High corrosion resistance against high temperature concentrated phosphoric acid.
（２）電気導電性がよいこと。(2) Good electrical conductivity.
（３） 薄板形状に容易に製作可能なこと。(3) It can be easily manufactured into a thin plate shape.
（４）積層構造に耐え得る強度があること。(4) Must have enough strength to withstand a laminated structure.
これらの特性に対する要求に対して、従来からセ’Ｚレ
ーター用部材としてカーボン板が用いられておシ、カー
ボン板を可能な限シ薄く加工して上記りん酸型燃料電池
用セルのセパレーターとして使用していた。In order to meet the demands for these characteristics, carbon plates have traditionally been used as separator members, and carbon plates have been processed to be as thin as possible and used as separators for the above-mentioned phosphoric acid fuel cells. Was.
上記カーボン板は、りん酸型燃料電池用セパレーターと
して優れた部材であるものの、もろい材料であるため、
カーボン板を薄く加工することが難しく、また取扱い中
に割れやすいという欠点があった。Although the above carbon plate is an excellent member as a separator for phosphoric acid fuel cells, it is a brittle material, so
It was difficult to process the carbon plate to be thin, and it also had the disadvantage that it was easily broken during handling.
ところが、一方では、シん酸型燃料電池には、第１図に
示されるようなカーボン板製上ノξレータ−１を含むス
タックセルが１例えば２００層も積層して用いられるた
め、セルを構成する部品の厚さが大きいと、りん酸型燃
料電池は大型となってしまうので、セルを構成する各部
品に対する薄肉化の要求が強く、セパレーターにも同じ
要求があるが、カーボン板では割れやすいという問題か
ら厚さは１ｍｌ程度が限界であった。However, on the other hand, in a cynic acid fuel cell, as many as 200 stacked cells (for example, 200 layers) each including a carbon plate upper ξlator 1 as shown in FIG. 1 are used. If the constituent parts are thick, the phosphoric acid fuel cell will become large, so there is a strong demand for thinning of each part that makes up the cell, and the same demand is also placed on the separator, but carbon plates are prone to cracking. The thickness was limited to about 1 ml due to the problem of being easy to use.
そこで、本発明者等は、上記りん酸型燃料電池用セルを
構成する部品の一部であるセパレーターを、従来のカー
ボン板よシも、薄く加工でき、高温濃縮シん酸に対する
耐食性が高く、電気導電性がよく、積層構造に耐える強
度を有する特性を兼ね備えた部材で製造すべく研究を行
った結果、（１）Ｔａ：１〜ｌＯ原子俤、
Ｐ：１５〜２３原子％、
残部：Ｎｌおよび不可避不純物。Therefore, the present inventors have realized that the separator, which is a part of the components constituting the above-mentioned phosphoric acid fuel cell, can be made thinner than the conventional carbon plate, and has high corrosion resistance against high-temperature concentrated phosphoric acid. As a result of conducting research to manufacture a member with characteristics that have good electrical conductivity and strength that can withstand a laminated structure, we found that (1) Ta: 1 to 10 atomic %, P: 15 to 23 atomic %, balance: Nl and unavoidable impurities.
からなるアモルファス合金、または。an amorphous alloy consisting of or.
（２） Ｔａ： １〜ｌ Ｏ原子％、Ｐ：１５〜２３
原子チ、
Ｂ、Ｓｉの１種または２穐二０．１〜７．０原子チを、
Ｐ−４−Ｂ＋Ｓｉ：１５〜２３原子チとなるように含有
し、
残部：Ｎ１および不可避不純物。(2) Ta: 1-1 O atom%, P: 15-23
Contains 0.1 to 7.0 atoms of one or two of B and Si such that P-4-B+Si: 15 to 23 atoms, remainder: N1 and inevitable impurities.
からなるアモルファス合金、
から作製することによシ、すぐれたりん酸型燃料電池用
セパレーターが得られるという知見を得たのである。They found that an excellent separator for phosphoric acid fuel cells can be obtained by manufacturing an amorphous alloy consisting of the following.
この発明は、かかる知見にもとづいてなされたものであ
って、上記（１）および（２）の合金で作製したりん酸
型燃料電池用セパレーターに特徴を有するものである。The present invention was made based on this knowledge, and is characterized by a separator for phosphoric acid fuel cells made of the alloys (1) and (2) above.
つぎに、この発明のシん酸型燃料電池用セ）Ｚレータ−
に用いるアモルファス合金の成分組成を上記の如く限定
した理由について述べる。Next, the Z-lator for cynic acid fuel cells of this invention
The reason for limiting the composition of the amorphous alloy used in the above-mentioned manner will be described below.
Ｔａ。Ta.
Ｔａは、保護皮膜を形成して耐食性を担う元素であるが
％ ２％ あるいは、ＰとＢおよびＳｌの少なくとも一
種と共存する場合は、ＰがＴａによる保護皮膜の形成を
加速するため、 Ｔａが１原子優でも保護皮膜が形成さ
れるが、 Ｔａが１０原子チを越えてもアモルファス形
成能が落ちて効果がない。Ta is an element that forms a protective film and plays a role in corrosion resistance. A protective film can be formed even if Ta exceeds 10 atoms, but the ability to form an amorphous layer decreases and there is no effect if Ta exceeds 10 atoms.
したがって、Ｔａの含有量を１〜１０原子チと定めた。Therefore, the Ta content was determined to be 1 to 10 atoms.
Ｐは、Ｎｉと共存してアモルファス構造を形成するのに
有効な作用かあり、Ｔａと共存してアモルファス構造を
形成するが、その含有量が１５原子−未満では、アモル
ファス形成能が低下し、２３原子チを越えて含有すると
高温濃シん酸中の環境で保護性の低いりん酸塩皮膜が生
じるので好ましくない。P has an effective effect in coexisting with Ni to form an amorphous structure, and coexisting with Ta to form an amorphous structure, but if its content is less than 15 atoms, the ability to form an amorphous decreases. If the content exceeds 23 atoms, a phosphate film with low protection properties will be formed in the environment of high-temperature concentrated citric acid, which is not preferable.
したがって、Ｐの含有量は、１５〜２３原子チと定めた
。Therefore, the content of P was determined to be 15 to 23 atoms.
８％Ｓｉ
ＢおよびＳｉ成分も、Ｎ１と共存してアモルファス構造
を形成するに有効な成分であシ、Ｐと置換可能な元素で
あるが、アモルファス形成能を高めるためには、Ｂ、Ｓ
ｉの１種または２種は最低０．１原子チは必要であシ、
また保護皮膜の形成を促すＰの作用を低下させないため
にはＢ 、 Ｓｉの１種または２種は７原子俤を越えて
含有してはならない。8%Si B and Si components are also effective components to coexist with N1 to form an amorphous structure, and are elements that can be substituted for P.
One or two types of i must have at least 0.1 atoms,
Furthermore, in order not to reduce the effect of P that promotes the formation of a protective film, one or both of B and Si must not be contained in an amount exceeding 7 atoms.
したがって、Ｂ、８ｉの１種または２穐の含有量を０．
１〜７．０原子チと定めた。Therefore, the content of one or both of B and 8i is set to 0.
It was determined to be 1 to 7.0 atoms.
Ｐ−１−Ｂ−１−８ｉ。P-1-B-1-8i.
ＢおよびＳｉ成分は、上述のようにＮｉと共存してアモ
ルファス構造を形成するのに有効であるが。B and Si components are effective in coexisting with Ni to form an amorphous structure as described above.
Ｐの一部と置換することにより一部アモルファス形成能
を高める作用もある。ところが、Ｐ、！：Ｂと８１の合
計が１５原子俤未満では、アモルファス形成能が低下し
耐食性も低下する。一方、ＰとＢと８１の合計が２３原
子俤を越えて含有すると保護皮膜の形成能が悪く耐食性
が低下する。したがって。By substituting a part of P, it also has the effect of partially enhancing the amorphous formation ability. However, P! : If the total amount of B and 81 is less than 15 atoms, the ability to form an amorphous layer decreases and the corrosion resistance also decreases. On the other hand, if the total amount of P, B, and 81 exceeds 23 atoms, the ability to form a protective film will be poor and the corrosion resistance will be reduced. therefore.
ＰとＢと８１の合計は、１５〜２３原子チと定めた。The total of P, B, and 81 was determined to be 15 to 23 atoms.
つぎに、この発明を実施例にもとづいて具体的に説明す
る。Next, the present invention will be specifically explained based on examples.
第１表に示される成分２組成を有する原料金属を混合し
、アルゴンアーク溶解炉により原料合金をつくり、これ
らの合金をアルゴン雰囲気中で再溶解し、単ロール法を
用いて超急冷凝固させることにより、厚さ：０．０５１
１１．幅：１００のアモルファス合金帯状薄板を得た。Mix raw material metals having the two component compositions shown in Table 1, create raw material alloys in an argon arc melting furnace, remelt these alloys in an argon atmosphere, and ultra-rapidly solidify them using a single roll method. Therefore, thickness: 0.051
11. An amorphous alloy strip thin plate having a width of 100 mm was obtained.
アモルファス構造の形成の確認は、Ｘ線回析によシ行っ
た。The formation of an amorphous structure was confirmed by X-ray diffraction.
これらアモルファス合金帯状薄板を、長さ：２００１１
３１に切断して、厚さ二〇、０５朋×幅＝１０顛×長さ
：２００に１にの薄板とし、この薄板の表面をシリコン
カーバイド紙１０００番迄シクロヘキサン中で研摩して
本発明セパレーター１〜７および比較セパレーター１〜
６を作製した。These amorphous alloy strip-shaped thin plates were made with length: 20011
The separator of the present invention was prepared by cutting the thin plate into 31 pieces with a thickness of 20.05 x width = 10 size x length: 200 to 1. The surface of this thin plate was polished in cyclohexane to silicon carbide paper No. 1000. 1 to 7 and comparison separator 1 to
6 was produced.
さらに、カーボン板を機械加工することによシ。Furthermore, by machining the carbon plate.
厚さ＝１０×幅：２５１！ＩＥＸ長さ：５００のカーボ
ン薄板を作製し、従来のカーボンセパレーターとした。Thickness = 10 x Width: 251! A carbon thin plate with an IEX length of 500 was produced and used as a conventional carbon separator.
これら、本発明セパレーター１〜７．比較セパレーター
１〜６および従来のカーボンセパレーターの比抵抗値を
測定した後、温度二１６０℃、濃度二８７重量％のＨ３
ＰＯ４溶液中に８日間浸漬し、単位時間および単位面積
当りの腐食によるセパレーターの重量減少量を測定した
。These separators of the present invention 1 to 7. After measuring the specific resistance values of comparative separators 1 to 6 and conventional carbon separators, H3 at a temperature of 160°C and a concentration of 287% by weight was
The separator was immersed in a PO4 solution for 8 days, and the weight loss of the separator due to corrosion per unit time and unit area was measured.
このようにして測定した値を、比較しやすくするために
、従来のカーボンセ・ξレーターの測定値に対する本発
明セパレーターおよび比較セ・ζレータ−の割合を、上
記カーボンセパレーター測定値】、００に対する割合と
して第１表に示した。In order to make it easier to compare the values measured in this way, the ratio of the separator of the present invention and the comparison separator to the measured value of the conventional carbon separator is calculated as follows: It is shown in Table 1 as follows.
第１表において、※印は、この発明の成分組成の条件を
外れた値を示すものである。In Table 1, the * mark indicates a value outside the conditions of the component composition of this invention.
なお、この実施例では、アモルファス合金の製造を単ロ
ール法で行ったが、この発明におけるアモルファス合金
の製造は、単ロール法のみに限定されるものではない。In this example, the amorphous alloy was produced by a single roll method, but the production of the amorphous alloy in this invention is not limited to the single roll method.
第１表に示された結果から明らかなように、この発明の
条件をみたすアモルファス合金で作製したセパレーター
は、従来のカーボンセパレーターと比べて高温濃りん酸
に対する耐食性がやや劣るが十分使用に耐え、電気抵抗
は小さく、また、板厚はアモルファス合金薄板から作製
するから機械加工を施すことなく極めて薄くすることが
可能であシ、靭性にもすぐれている。As is clear from the results shown in Table 1, separators made of amorphous alloys that meet the conditions of the present invention have slightly lower corrosion resistance against high-temperature concentrated phosphoric acid than conventional carbon separators, but can withstand use sufficiently. It has low electrical resistance, and since it is made from an amorphous alloy thin plate, it can be made extremely thin without machining, and it has excellent toughness.
したがって、この発明のセパレーターをシん酸型燃料電
池に使用することによ９１強度のある小型のりん酸型燃
料電池をつくることができるというすぐれた効果を奏す
るものである。Therefore, by using the separator of the present invention in a phosphoric acid fuel cell, it is possible to produce a small phosphoric acid fuel cell having a strength of 91, which is an excellent effect.
第１図は、りん酸型燃料電池のセルの概略図である。
１・・・セパレーター、 ２・・・負極、３・・・
電極触媒、 ４・・・電解質、５・・・正極。FIG. 1 is a schematic diagram of a phosphoric acid fuel cell. 1...Separator, 2...Negative electrode, 3...
Electrode catalyst, 4... Electrolyte, 5... Positive electrode.
Claims (2)
りん酸型燃料電池用セパレーター。(1) A separator for a phosphoric acid fuel cell, characterized in that it is made of an amorphous alloy consisting of Ta: 1 to 10 atomic %, P: 15 to 23 atomic %, and the remainder: Ni and inevitable impurities.
りん酸型燃料電池用セパレーター。(2) Ta: 1 to 10 at%, P: 15 to 23 at%, one or both of B and Si: 0.1 to 7.0 at%, P+B+Si: 15 to 23 at% 1. A separator for a phosphoric acid fuel cell, characterized in that it is made of an amorphous alloy comprising: Ni and unavoidable impurities.
Priority Applications (7)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62111467A JPS63277736A (en) | 1987-05-07 | 1987-05-07 | Separator for phosphoric acid type fuel cell |
| KR1019890700011A KR940004900B1 (en) | 1987-05-07 | 1988-05-07 | Highly corrosion-resistant amorphous alloy |
| PCT/JP1988/000449 WO1988008885A1 (en) | 1987-05-07 | 1988-05-07 | Highly corrosion-resistant amorphous alloy |
| EP88903960A EP0314805B1 (en) | 1987-05-07 | 1988-05-07 | Highly corrosion-resistant amorphous nickel-based alloy |
| DE3853190T DE3853190T2 (en) | 1987-05-07 | 1988-05-07 | HIGH CORROSION-RESISTANT AMORPHOUS ALLOY. |
| FI890031A FI98074C (en) | 1987-05-07 | 1989-01-04 | Amorphous nickel alloy for use in corrosive environments |
| US07/914,027 US5634989A (en) | 1987-05-07 | 1992-07-15 | Amorphous nickel alloy having high corrosion resistance |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP62111467A JPS63277736A (en) | 1987-05-07 | 1987-05-07 | Separator for phosphoric acid type fuel cell |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPS63277736A true JPS63277736A (en) | 1988-11-15 |
Family
ID=14561983
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP62111467A Pending JPS63277736A (en) | 1987-05-07 | 1987-05-07 | Separator for phosphoric acid type fuel cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS63277736A (en) |
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2005294102A (en) * | 2004-04-01 | 2005-10-20 | Dainatsukusu:Kk | Method of manufacturing metal glass separator |
| WO2006059402A1 (en) * | 2004-12-03 | 2006-06-08 | Dynax Corporation | Method of manufacturing metal glass separator |
-
1987
- 1987-05-07 JP JP62111467A patent/JPS63277736A/en active Pending
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2005294102A (en) * | 2004-04-01 | 2005-10-20 | Dainatsukusu:Kk | Method of manufacturing metal glass separator |
| WO2006059402A1 (en) * | 2004-12-03 | 2006-06-08 | Dynax Corporation | Method of manufacturing metal glass separator |
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