JPS60216458A - Regeneration method of negative electrode of high-temperature fuel cell - Google Patents
Regeneration method of negative electrode of high-temperature fuel cellInfo
- Publication number
- JPS60216458A JPS60216458A JP59071970A JP7197084A JPS60216458A JP S60216458 A JPS60216458 A JP S60216458A JP 59071970 A JP59071970 A JP 59071970A JP 7197084 A JP7197084 A JP 7197084A JP S60216458 A JPS60216458 A JP S60216458A
- Authority
- JP
- Japan
- Prior art keywords
- anode
- gas
- fuel cell
- control valve
- cell
- 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.)
- Granted
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
- H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
- H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
- H01M8/2425—High-temperature cells with solid 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
- H01M8/04223—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids during start-up or shut-down; Depolarisation or activation, e.g. purging; Means for short-circuiting defective fuel cells
-
- 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
- H01M8/0297—Arrangements for joining electrodes, reservoir layers, heat exchange units or bipolar separators to each other
-
- 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
- H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
- H01M8/241—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes
- H01M8/244—Grouping of fuel cells, e.g. stacking of fuel cells with solid or matrix-supported electrolytes with matrix-supported molten electrolyte
-
- 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)
- Inert Electrodes (AREA)
- Fuel Cell (AREA)
Abstract
Description
【発明の詳細な説明】
産業上の利用分野
本発明は、動作温度が比較的高く、負極（アノード）材
料として金属を用いた高温燃料電池に関するもので、特
に溶融炭酸塩燃料電池のアノード再生法に関係するもの
である。DETAILED DESCRIPTION OF THE INVENTION Field of the Invention The present invention relates to high-temperature fuel cells with relatively high operating temperatures and using metal as the negative electrode (anode) material, and in particular to an anode regeneration method for molten carbonate fuel cells. It is related to.
従来例の構成とその問題点
従来、高温燃料電池の代表的なものとして溶融炭酸塩燃
料電池や固体電解質燃料電池などが知られているが、高
温であることなど条件が厳しいた２ ぺ−１ｌ
めに材料面での制約が大きい。その中で溶融炭酸塩燃料
電池は動作温度が約６６０°Ｃと、金属材料が使用でき
る温度領域であるため、マウント関係およびアノードな
どには金属が用いられている。Structures of conventional examples and their problems Conventionally, molten carbonate fuel cells and solid electrolyte fuel cells have been known as typical high-temperature fuel cells, but they have difficult conditions such as high temperatures. Therefore, there are major restrictions in terms of materials. Among these, molten carbonate fuel cells have an operating temperature of about 660° C., which is a temperature range in which metal materials can be used, so metal is used for the mounts, anodes, and the like.
溶融炭酸′塩燃刺電池のアノードとしてはニッケル微粉
末を焼結した多孔板などが用いられているが、水素を主
成分どする還元性のアノードガス雰囲気下で長時間６５
０°Ｃの温度に保たれるため、ニッケル微粉末の焼結が
進行し、アノードの多孔度が低下するという問題が生じ
ていた。ニッケル多孔板の焼結が進行し、多孔度が減少
すると、反応に関与できる電極面積が減少し、アノード
の性能が低下するため、電池としての寿命が低下するこ
とになる。A porous plate made of sintered fine nickel powder is used as the anode of a molten carbonate burning battery, but it is not possible to use it for a long time in an atmosphere of reducing anode gas containing hydrogen as the main component.
Since the temperature is maintained at 0°C, sintering of the fine nickel powder progresses, causing a problem that the porosity of the anode decreases. As the sintering of the nickel porous plate progresses and the porosity decreases, the area of the electrode that can participate in the reaction decreases, and the performance of the anode deteriorates, resulting in a shortened battery life.
このアノードの焼結進行を抑制するため、従来いくつか
の方法が考えられてきた。その１つにはアノード材料の
ニッケルに、高融点金属成分、たとえばクロム、ジルコ
ニウム々どを添加して焼結進行を抑える方法がある。そ
のほかニッケル粉末にアルミナなどのセラミックス微粉
末を混入する３ぺ−１
方法や、セラミクス粒子表面にニッケルメッキを施し、
このメタルコートセラミクス粒子でアノードを構成する
などの方法が考えられてきている。Several methods have been considered in the past to suppress the progress of sintering of the anode. One method is to suppress the progress of sintering by adding high melting point metal components such as chromium and zirconium to the nickel of the anode material. In addition, there is a 3-P1 method in which fine ceramic powder such as alumina is mixed into nickel powder, and nickel plating is applied to the surface of ceramic particles.
Methods such as forming an anode using these metal-coated ceramic particles have been considered.
とれらの方法は一応の効果があり、アノードの焼結進行
がかなり抑えられる事がわがっている。It is known that these methods are somewhat effective and can considerably suppress the progress of sintering of the anode.
しかし、それでもなお焼結の進行により、電池性能は数
千時間の運転中に徐々に低下していく。従って燃料電池
が寿命として要求されている致方時間の間、アノードが
前述のような方法だけでその性能を維持することは不可
能であった。However, due to the progress of sintering, cell performance gradually deteriorates over thousands of hours of operation. Therefore, it has been impossible for the anode to maintain its performance only in the above-described manner during the required lifetime of the fuel cell.
発明の目的
そこで本発明は、長時間の運転期間中に焼結が進行し、
多孔度、比表面積などが低下したアノードを電池に組み
込まれた状態のまま再生処理し、その寿命を大きく伸ば
す事を目的とする。Purpose of the Invention Therefore, the present invention aims to provide a method in which sintering progresses during a long period of operation.
The purpose is to recycle anodes with reduced porosity, specific surface area, etc. while still being incorporated into batteries, thereby greatly extending their lifespan.
発明の構成
本発明は、金属または金属とセラミクスからなる多孔質
アノードを構成要素とする高温燃料電池において、アノ
ードを酸化させ、ついで還元する工程を加えることを特
徴とするものである。その好捷しい手段としては一般に
は燃オ」電池を無負荷の状態にしてから、アノードガス
の供給を市め、不活性ガスによってアノードガスをパー
ジした後、カソードガスまたｄ他の酸化性ガスを供給し
アノードを構成する金属成分を酸化する。その後再び不
活性ガスによるパージに続くアノードガスまたは他の還
元性ガスを供給して、アノードを再生させる各工程から
成る高温燃料電池のアノード再生法である。Structure of the Invention The present invention is a high-temperature fuel cell having a porous anode made of metal or metal and ceramics, which is characterized by adding a step of oxidizing the anode and then reducing it. A preferred method is generally to put the fuel cell in an unloaded state, then turn on the anode gas, purge the anode gas with an inert gas, and then remove the cathode gas or other oxidizing gas. oxidizes the metal components that make up the anode. This is an anode regeneration method for a high-temperature fuel cell, which consists of steps of purging with an inert gas and then supplying an anode gas or other reducing gas to regenerate the anode.
実施例の説明
第１図に本発明の実施例におけるガス系統の概略図を示
す。１ｄ、燃料電池、２はアノードガス供給源、３はカ
ソードガス供給源であり、アノードガス及びカソードガ
スはそれぞれ調節弁４，５を介して電池のアノード室及
びカソード室へ供給されるようになっている。６はパー
ジガス供給源であり、アノードガス供給系統にはパージ
ガス調節弁７．酸化性ガス（ここではカソードガス）調
節弁８を介してパージガスおよび酸化性ガスが供給され
るようになっている。なお、本実施例におい６ 〈 ；
゛
ては燃料電池として溶融炭酸塩燃料電池を用いており、
酸化性ガスとしてはカソードガス（空気と二酸化炭素の
混合物）をそのまま使用する形となっている。また還元
性ガスとしては、水素を主成分としているアノードガス
をそのまま用い、パージガスとしてはボンベ供給の窒素
ガスを用いている。−！、たここで用いた溶融炭酸塩燃
料電池は、約、２０ｆｆｉ角の大きさの単電池を４セル
積層したもので、アノードとしてはクロムを１ｄ重量％
含有するニッケル焼結多孔体を用いた。！た電池は８５
０°Ｃで運転させた。DESCRIPTION OF EMBODIMENTS FIG. 1 shows a schematic diagram of a gas system in an embodiment of the present invention. 1d is a fuel cell; 2 is an anode gas supply source; 3 is a cathode gas supply source; anode gas and cathode gas are supplied to the anode chamber and cathode chamber of the cell through control valves 4 and 5, respectively; ing. 6 is a purge gas supply source, and the anode gas supply system includes a purge gas control valve 7. Purge gas and oxidizing gas are supplied through an oxidizing gas (cathode gas here) control valve 8 . Note that in this example 6 <;
One uses a molten carbonate fuel cell as a fuel cell,
The cathode gas (a mixture of air and carbon dioxide) is used as is as the oxidizing gas. Further, as the reducing gas, an anode gas containing hydrogen as a main component is used as is, and as the purge gas, nitrogen gas supplied from a cylinder is used. -! The molten carbonate fuel cell used here is a stack of four single cells with a size of approximately 20ffi square, and the anode contains 1dwt% chromium.
A sintered porous body containing nickel was used. ! The battery is 85
It was operated at 0°C.
電池の初期性能は１００ｍム／ｄの負荷で１セル当りの
出力電圧が０．８６ Ｖであった。これを同一負荷のも
とて連続運転したところ、第２図に示すように３０００
時間を経過した時点で出力電圧は１セル当り０．８２
Ｖに低下していた。The initial performance of the battery was an output voltage of 0.86 V per cell at a load of 100 mm/d. When this was operated continuously under the same load, as shown in Figure 2, 3000
As time passes, the output voltage is 0.82 per cell.
It had dropped to V.
そこで、アノードの再生を行なうため次の操作を行なっ
た。まず電池から負荷をはずし、パージガス調節弁７を
開けると同時にアノードガス調節弁４を閉じる。３分間
パージガス（窒素ガス）を６ く 。Therefore, the following operation was performed to regenerate the anode. First, the load is removed from the battery, and at the same time the purge gas control valve 7 is opened, the anode gas control valve 4 is closed. Apply purge gas (nitrogen gas) for 3 minutes.
流し、内？Ｔ（５のアノードガスを追い出した後、パー
ジガス調節弁７を閉じると同時に酸化性ガス調節弁８を
開けて酸化性ガスであるカソードガスを供給した。この
時点で電池の出力電圧は０．２〜ＯＶの電圧しか示さず
、アノードのニッケル焼結多孔体は酸化され、酸化ニッ
ケルと化す。約２時間酸化性ガスを流した後、前述と逆
の手順で酸化性ガスを止めてパージガスを流し、再びア
ノードガス調節弁４を開けて還元性ガスとしてのアノー
ドガスに切シ替える。還元性ガスを流すと同時に電池出
力電圧は上昇し始めるが、酸化されたアノードを完全に
還元するため、このまま無弁待状態で２時間保持した。Inside the sink? After expelling the anode gas at T (5), the purge gas control valve 7 was closed, and at the same time the oxidizing gas control valve 8 was opened to supply cathode gas, which is an oxidizing gas.At this point, the output voltage of the battery was 0.2 The sintered nickel porous body of the anode is oxidized and turns into nickel oxide.The nickel sintered porous body of the anode shows only a voltage of ~OV.After flowing the oxidizing gas for about 2 hours, stop the oxidizing gas and flow the purge gas in the reverse order as described above. , open the anode gas control valve 4 again and switch to the anode gas as a reducing gas.At the same time as the reducing gas flows, the battery output voltage begins to rise, but in order to completely reduce the oxidized anode, it remains as it is. It was held for 2 hours without any warning.
その後、電池に負荷をつ々ぎ、徐々に負荷を増していっ
たところ、約３時間後には１ｄｏｍＡ／ＣＪの負荷にお
いて１セル当りの出力電圧が０．８５Ｖを示し、初期性
能に近い性能にまで回復したことが確認された。After that, we gradually increased the load on the battery, and after about 3 hours, the output voltage per cell showed 0.85V at a load of 1domA/CJ, and the performance was close to the initial performance. It was confirmed that he had recovered.
このような性能の回復はアノードの再生によるものであ
って、その理由については以下のように考えられる。す
なわち、長時間の使用により焼結了（−゛
が進行し、多孔度と比表面積が減少したアノードを、一
度完全に酸化し、それを再び還元することによりアノー
ドの表面が微視的に荒らされ、また酸化過程での体積変
化によるクラック発生もあるため、多孔度と比表面積が
一部回復するだめと考えられる。This recovery in performance is due to the regeneration of the anode, and the reason is considered as follows. In other words, the anode, which has undergone sintering (-) due to long-term use and reduced porosity and specific surface area, is completely oxidized and then reduced again, so that the surface of the anode becomes microscopically rough. In addition, cracks may occur due to volume changes during the oxidation process, so it is thought that the porosity and specific surface area cannot be partially recovered.
このことを検証するため、前記アノードを使用前（Ａ）
、水素気流中６５０’Ｃで２０００時間放置（Ｂ）。In order to verify this, the anode was tested before use (A).
, left for 2000 hours at 650'C in a hydrogen stream (B).
Ｂのザンプルを前記実施例同様６６０°Ｃで空気酸化し
た後、再び水素還元（Ｃ）の３つの処理をし、それぞれ
について水銀圧入ポロシメータによる多孔度および平均
孔径の測定を行なった。次表にその結果を示す。After the sample B was air oxidized at 660°C as in the previous example, it was again subjected to three treatments of hydrogen reduction (C), and the porosity and average pore diameter of each sample were measured using a mercury intrusion porosimeter. The results are shown in the table below.
この結果から、焼結が進んだアノードに酸化還元処理を
施すと多孔度などがかなり回復することが確認できる。From this result, it can be confirmed that porosity etc. can be considerably recovered when the sintered anode is subjected to redox treatment.
なお、実施例においては、酸化性ガスとしてカソードガ
スを用い、還元性ガスとしてアノードガスを用いたが、
これらはもちろん他の純ガスまたは混合ガスであっても
良く、供給手段もたとえばボンベを用いても良い。また
再生操作における各ガスを供給する時間については電池
の規模、ガス流量により異なってくる。さらに実施例に
おいては高温燃料電池として溶融炭酸塩燃料電池を用い
ているが、焼結が進むことにより性能が低下し、これを
酸化、還元することにより抑制できる系においては他の
タイプのものであっても良い。In addition, in the examples, cathode gas was used as the oxidizing gas and anode gas was used as the reducing gas, but
These may of course be other pure gases or mixed gases, and the supply means may also be, for example, cylinders. Further, the time for supplying each gas in the regeneration operation varies depending on the scale of the battery and the gas flow rate. Furthermore, although a molten carbonate fuel cell is used as a high-temperature fuel cell in the example, performance deteriorates as sintering progresses, and other types of fuel cells may be used in systems where this can be suppressed by oxidation or reduction. It's okay.
発明の効果
以上のように、本発明によれば、電池を分解することな
く簡単な操作で焼結が進行したアノードを再生すること
ができ、初期性能に近いところにまで電池性能を回復す
ることができる。従ってアノードの焼結進行により電池
性能が低下した際に本♀明の再生法を実施すれば、電池
の寿命を太き９ ページ
く引き伸ばすことが可能となる。Effects of the Invention As described above, according to the present invention, a sintered anode can be regenerated by a simple operation without disassembling the battery, and the battery performance can be restored to a level close to the initial performance. I can do it. Therefore, if the regeneration method of the present invention is implemented when the battery performance deteriorates due to the progress of sintering of the anode, the life of the battery can be extended by 9 pages.
第１図は本発明によるアノード再生法を実施するだめの
１つのガス系統概略図、第２図は実施例における電池性
能の経時変化図である。
１・・・・・・燃料電池、２・・・・・・アノードガス
供給源、３・・・・・・カソードガス供給源、４，６．
了・・・・・・調節弁、６・・・１、・パージガス供給
源。
代理人の氏名 弁理士 中 尾 敏 男 ほか１名３１
３FIG. 1 is a schematic diagram of one gas system for carrying out the anode regeneration method according to the present invention, and FIG. 2 is a graph of changes in battery performance over time in an example. 1... Fuel cell, 2... Anode gas supply source, 3... Cathode gas supply source, 4, 6.
Completed...Control valve, 6...1, Purge gas supply source. Name of agent: Patent attorney Toshio Nakao and 1 other person31
3
Claims (1)
要素とする高温燃料電池の負極の再生法であって、前記
負極へ酸化性ガスを供給ｌ〜て負極の構成金属成分を酸
化し、その後還元性ガスを供給することにより、負極を
還元再生させることを特徴とする高温燃料電池の負極の
再生法。A method for regenerating a negative electrode of a high-temperature fuel cell comprising a porous negative electrode made of metal or metal and ceramics, the method comprises: supplying an oxidizing gas to the negative electrode to oxidize the constituent metal components of the negative electrode; A method for regenerating a negative electrode of a high-temperature fuel cell, characterized by reductively regenerating the negative electrode by supplying gas.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59071970A JPS60216458A (en) | 1984-04-11 | 1984-04-11 | Regeneration method of negative electrode of high-temperature fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP59071970A JPS60216458A (en) | 1984-04-11 | 1984-04-11 | Regeneration method of negative electrode of high-temperature fuel cell |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| JPS60216458A true JPS60216458A (en) | 1985-10-29 |
| JPH0521311B2 JPH0521311B2 (en) | 1993-03-24 |
Family
ID=13475832
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP59071970A Granted JPS60216458A (en) | 1984-04-11 | 1984-04-11 | Regeneration method of negative electrode of high-temperature fuel cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPS60216458A (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| NL8801797A (en) * | 1987-01-09 | 1990-02-01 | New Energy And Ind Technology | FUEL CELL WITH MELTED CARBONATE AND METHOD FOR CONTROLLING THEIR OPERATION |
| WO1995025588A1 (en) * | 1994-03-21 | 1995-09-28 | British Technology Group Limited | Porous metal composite body |
| WO2011052283A1 (en) * | 2009-10-29 | 2011-05-05 | コニカミノルタホールディングス株式会社 | Fuel cell device |
| KR101894043B1 (en) * | 2017-08-30 | 2018-08-31 | 고등기술연구원연구조합 | Post-treatment apparatus of solid oxide fuel cell stack and post-treatment method thereof |
-
1984
- 1984-04-11 JP JP59071970A patent/JPS60216458A/en active Granted
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| NL8801797A (en) * | 1987-01-09 | 1990-02-01 | New Energy And Ind Technology | FUEL CELL WITH MELTED CARBONATE AND METHOD FOR CONTROLLING THEIR OPERATION |
| WO1995025588A1 (en) * | 1994-03-21 | 1995-09-28 | British Technology Group Limited | Porous metal composite body |
| US5798148A (en) * | 1994-03-21 | 1998-08-25 | British Technology Group Limited | Porous metal composite body |
| WO2011052283A1 (en) * | 2009-10-29 | 2011-05-05 | コニカミノルタホールディングス株式会社 | Fuel cell device |
| JP4821937B2 (en) * | 2009-10-29 | 2011-11-24 | コニカミノルタホールディングス株式会社 | Fuel cell device |
| KR101894043B1 (en) * | 2017-08-30 | 2018-08-31 | 고등기술연구원연구조합 | Post-treatment apparatus of solid oxide fuel cell stack and post-treatment method thereof |
Also Published As
| Publication number | Publication date |
|---|---|
| JPH0521311B2 (en) | 1993-03-24 |
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