JPH0714592A - Regenerating method for molten carbonate fuel cell - Google Patents
Regenerating method for molten carbonate fuel cellInfo
- Publication number
- JPH0714592A JPH0714592A JP5177594A JP17759493A JPH0714592A JP H0714592 A JPH0714592 A JP H0714592A JP 5177594 A JP5177594 A JP 5177594A JP 17759493 A JP17759493 A JP 17759493A JP H0714592 A JPH0714592 A JP H0714592A
- Authority
- JP
- Japan
- Prior art keywords
- cathode
- electrolyte
- gas
- fuel cell
- molten carbonate
- 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
-
- 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)
Abstract
Description
【０００１】[0001]
【産業上の利用分野】本発明は燃料の有する化学エネル
ギーを直接電気エネルギーに変換するエネルギー部門で
用いる燃料電池のうち、溶融炭酸塩型燃料電池の電解質
が減少して性能が劣化したときに再生させる再生方法に
関するものである。BACKGROUND OF THE INVENTION The present invention relates to a fuel cell used in the energy sector for directly converting chemical energy of a fuel into electric energy, and regenerated when the performance of a molten carbonate fuel cell is deteriorated due to a decrease in electrolyte. The present invention relates to a reproducing method for making it.
【０００２】[0002]
【従来の技術】燃料電池のうち、溶融炭酸塩型燃料電池
は、図２に一例の概略を示す如く、電解質として炭酸塩
を溶融させて多孔質体にしみ込ませてなる電解質板（タ
イル）１をカソード（酸素極）２とアノード（燃料極）
３の両電極で両面から挟んだセルをセパレータ４を介し
て積層し、カソード２側に形成したガス通路５に酸化ガ
ス（空気、ＣＯ2 ）ＯＧを、又、アノード３側に形成し
たガス通路６に燃料ガス（Ｈ2 ）ＦＧをそれぞれ供給す
ることによりカソード２側とアノード３側で電気化学反
応を起こさせることにより発電するようにしたものを、
図示しない締付装置にて締め付けてカソード２とアノー
ド３を電解質板１に密着させるようにしてある。2. Description of the Related Art Among fuel cells, a molten carbonate fuel cell is an electrolyte plate (tile) 1 made by melting carbonate as an electrolyte and impregnating it into a porous body, as shown schematically in FIG. The cathode (oxygen electrode) 2 and the anode (fuel electrode)
The cells sandwiched by both electrodes of No. 3 from both sides are laminated via the separator 4, the oxidizing gas (air, CO 2 ) OG is provided in the gas passage 5 formed on the cathode 2 side, and the gas passage formed on the anode 3 side. 6, a fuel gas (H 2 ) FG is supplied respectively to cause an electrochemical reaction on the cathode 2 side and the anode 3 side to generate electric power.
The cathode 2 and the anode 3 are tightly attached to the electrolyte plate 1 by tightening with a tightening device (not shown).
【０００３】[0003]
【発明が解決しようとする課題】ところが、溶融炭酸塩
型燃料電池は、時間の経過とともに電解質が次第に減少
し、これにより電池の電圧が低下して性能が劣化して来
る問題がある。かかる問題を解決するためには、外部か
ら電解質を補給することが考えられるが、従来、実際に
は外部からの電解質の補給は行われていないので、溶融
炭酸塩型燃料電池を再生させることができなかった。However, the molten carbonate fuel cell has a problem that the electrolyte gradually decreases with the lapse of time, whereby the voltage of the cell is lowered and the performance is deteriorated. In order to solve such a problem, it is possible to replenish the electrolyte from the outside, but conventionally, since the electrolyte is not actually replenished from the outside, it is possible to regenerate the molten carbonate fuel cell. could not.
【０００４】そこで、本発明者は、溶融炭酸塩型燃料電
池の電解質板にしみ込ませた電解質が減少したときに外
部から電解質を補給することなく電池性能の劣化を回復
させて再生させるようにすることについて種々工夫研究
を重ねた結果、溶融炭酸塩型燃料電池のカソードは、使
用時に締付装置により付与される圧縮荷重によりクリー
プ変形することがないようにするため、素材として酸化
ニッケルＮｉＯが用いられていて、Ｎｉ粉を焼結した多
孔質体を電池に組み込み、運転中に酸化させてＮｉＯと
するようにしてあること、ＮｉＯは圧縮変形に耐え得る
が、Ｎｉは圧縮変形し易いこと、ＮｉＯを素材とするカ
ソードはＮｉ粉末焼結体が用いられているアノードと違
って濡れ性があって、通常、電解質が全体に対し５０％
位含浸していて、カソードは電解質中に漬っている状態
になっていること、等に着目し、カソードに含浸してい
る電解質を電解質板又はアノードへ再配分させれば、溶
融炭酸塩型燃料電池を再生させることができることを見
い出し本発明をなした。Therefore, the inventor of the present invention tries to recover and regenerate the deterioration of the cell performance without replenishing the electrolyte from the outside when the electrolyte soaked in the electrolyte plate of the molten carbonate fuel cell decreases. As a result of repeated research into various ideas, nickel oxide NiO was used as the material for the cathode of the molten carbonate fuel cell in order to prevent creep deformation due to the compressive load applied by the tightening device during use. That a porous body obtained by sintering Ni powder is incorporated into a battery and is oxidized during operation to NiO, NiO can withstand compressive deformation, but Ni easily compresses and deforms, A cathode made of NiO has wettability unlike an anode using a Ni powder sintered body, and the electrolyte is usually 50% of the whole.
If the electrolyte impregnated in the cathode is redistributed to the electrolyte plate or anode, paying attention to the fact that the cathode is immersed in the electrolyte and the cathode is immersed in the electrolyte. The present invention has been made by finding that the fuel cell can be regenerated.
【０００５】したがって、本発明は、溶融炭酸塩型燃料
電池の電解質が減少しても、外部から電解質を補給する
ことなく、カソード内部の電解質を電解質板、アノード
に配分させて電池の性能劣化を回復させるようにしよう
とするものである。Therefore, according to the present invention, even if the amount of electrolyte in the molten carbonate fuel cell decreases, the electrolyte inside the cathode is distributed to the electrolyte plate and the anode without replenishing the electrolyte from the outside, thereby deteriorating the performance of the cell. It tries to recover.
【０００６】[0006]
【課題を解決するための手段】本発明は、上記課題を解
決するために、カソードの素材としてＮｉ粉を焼結した
多孔質体の酸化物を用いた溶融炭酸塩型燃料電池を、そ
の運転温度下において、カソード側とアノード側に不活
性ガスを流した後、カソード側にＨ2 ガスを流してカソ
ードを還元してＮｉＯをＮｉとし、カソードの電解質に
対する濡れ性を低下させ、次いで、この状態で締付装置
にて電池全体を圧縮し、カソードを圧縮変形させて余剰
となったカソード内部の電解質をカソードから出して、
その電解質を電解質板とアノードに再配分し、しかる
後、カソード側に酸化ガスを流してカソードを酸化さ
せ、カソードの空隙を減少させることで、一度再配分さ
れた電解質が再びカソードに戻ることを制限する。In order to solve the above-mentioned problems, the present invention operates a molten carbonate fuel cell using a porous oxide of sintered Ni powder as a cathode material. At a temperature, after flowing an inert gas on the cathode side and the anode side, H 2 gas is caused to flow on the cathode side to reduce the cathode to NiO to Ni, thereby reducing the wettability of the cathode with respect to the electrolyte. In this state, the entire battery is compressed by the tightening device, the cathode is compressed and deformed, and the excess electrolyte inside the cathode is discharged from the cathode,
The electrolyte is redistributed between the electrolyte plate and the anode, and then the cathode is oxidized by flowing an oxidizing gas to the cathode side to reduce the voids in the cathode, so that the electrolyte once redistributed is returned to the cathode again. Restrict.
【０００７】[0007]
【作用】カソードを還元してＮｉＯからＮｉにすると、
カソードの電解質に対する濡れ性が低下すると同時にＮ
ｉは容易にクリープ変形するので、カソード還元後圧縮
変形させることによりカソードは変形させられて、カソ
ードの空隙が減少する。カソードの空隙が減少すると、
カソード内部に存在する電解質のうち余剰となった電解
質を電解質板及びアノードに再配分することができる。
これにより電解質を外部から補充することなく電池の性
能低下を回復させることができる。[Function] When the cathode is reduced to convert NiO to Ni,
At the same time that the wettability of the cathode to the electrolyte decreases
Since i easily undergoes creep deformation, the cathode is deformed by compressing and deforming after reducing the cathode, so that the voids in the cathode are reduced. As the cathode voids decrease,
It is possible to redistribute excess electrolyte out of the electrolyte existing inside the cathode to the electrolyte plate and the anode.
This makes it possible to recover the deterioration of the battery performance without replenishing the electrolyte from the outside.
【０００８】[0008]
【実施例】以下、本発明の実施例を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.
【０００９】図１は本発明の方法を実施する工程を示す
もので、図２に示した燃料電池スタックの場合と同様
に、電解質として溶融炭酸塩をしみ込ませた電解質板１
をカソード２とアノード３の両電極で両面から挟んでな
るセルをセパレータ４を介し多層に積層して、上記セパ
レータ４により形成されたカソード２側のガス通路５に
酸化ガス（空気、ＣＯ2 ）を供給すると共に、アノード
３側のガス通路６に燃料ガスＨ2 を供給して運転を行う
ようにしてある溶融炭酸塩型燃料電池において、電解質
が次第に減少して来て電池の電圧が低下して来ると、本
発明の方法で再生させる。FIG. 1 shows steps for carrying out the method of the present invention. Like the fuel cell stack shown in FIG. 2, an electrolyte plate 1 impregnated with molten carbonate as an electrolyte is shown.
Cells are sandwiched between the cathode 2 and the anode 3 from both sides, and are laminated in multiple layers via a separator 4, and an oxidizing gas (air, CO 2 ) is introduced into a gas passage 5 formed by the separator 4 on the cathode 2 side. In the molten carbonate fuel cell in which the fuel gas H 2 is supplied to the gas passage 6 on the side of the anode 3 to perform the operation, the electrolyte gradually decreases and the voltage of the cell decreases. When it comes, it is regenerated by the method of the present invention.
【００１０】この場合、電池の電圧低下が検知される
と、通常運転状態を停止させた後、運転温度を保持した
まま先ず、電池内を不活性ガスとしてのＮ2 ガスでパー
ジさせるため、図１（イ）の如く、各セルのカソード２
側のガス通路５及びアノード３側のガス通路６に不活性
ガスとしてＮ2 ガスを供給し、カソード２側の酸化ガス
（空気、ＣＯ2 ）、アノード３側の燃料ガスＨ2 とＮ2
とを置換させる。In this case, when the voltage drop of the battery is detected, the normal operation state is stopped, and then the inside of the battery is purged with N 2 gas as an inert gas while maintaining the operation temperature. Cathode 2 of each cell as shown in 1 (a)
Side gas passage 5 and anode 3 side gas passage 6 are supplied with N 2 gas as an inert gas, cathode 2 side oxidizing gas (air, CO 2 ), anode 3 side fuel gas H 2 and N 2
Replace and.
【００１１】次に、図１（ロ）の如く、カソード２側の
ガス通路５にＮ2 ガスとＨ2 ガスを流すことによりカソ
ード２を還元させ、素材のＮｉＯをＮｉにする。Next, as shown in FIG. 1B, the cathode 2 is reduced by flowing N 2 gas and H 2 gas into the gas passage 5 on the cathode 2 side, and NiO as a raw material is changed to Ni.
【００１２】ＮｉＯは電解質に対する濡れ性が良く、且
つクリープに強いが、Ｎｉは電解質に濡れにくく、且つ
容易にクリープ変形するので、この性質を利用して、素
材が変形し易いカソード還元状態のときに、図１（ハ）
に矢印で示す如く、図示しないスタック締付装置により
電池全体を圧縮させてカソード２を変形させる。これに
より、カソード２の容積が減少してカソードの空隙が減
少し、このカソードの空隙減少に伴い余剰となったカソ
ード内部の電解質が他の部分、すなわち、電解質板１、
アノード３に再配分されることになる。たとえば、カソ
ード２を還元させる前のカソード容積を１００％とし、
カソード還元後クリープ変形させて８０％に容積が減少
したとすると、通常カソード２に電解質が５０％存在し
ているとしたときに、上記カソード容積が１００％から
８０％に減少することに伴い電解質は５０％から４０％
でよいことになり、余剰となった１０％分の電解質が他
に利用できることになる。NiO has a good wettability with respect to the electrolyte and is strong against creep, but Ni is hard to get wet with the electrolyte and easily undergoes creep deformation. Therefore, by utilizing this property, when the material is in a cathode-reduced state where it is easily deformed. In addition, Fig. 1 (C)
As indicated by the arrow, the whole battery is compressed by a stack tightening device (not shown) to deform the cathode 2. As a result, the volume of the cathode 2 is reduced and the voids of the cathode are reduced, and the excess electrolyte inside the cathode due to the reduction of the voids of the cathode is the other part, that is, the electrolyte plate 1,
It will be redistributed to the anode 3. For example, assuming that the cathode volume before reducing the cathode 2 is 100%,
Assuming that the volume is reduced to 80% by creep deformation after the reduction of the cathode, and when the electrolyte normally exists in the cathode 2 at 50%, the above-mentioned cathode volume is reduced from 100% to 80%. Is 50% to 40%
This means that 10% of the surplus electrolyte can be used for other purposes.
【００１３】上記カソード還元状態でのカソード圧縮変
形が終ると、図１（ニ）に示す如く、カソード２側のガ
ス通路５にＮ2 ガスとともに酸化ガス（空気、ＣＯ2 ）
を流してカソード２を酸化させてクリープ変形に強いＮ
ｉＯとするようにし、アノード３側のガス通路６にはＮ
2 ガスとともに燃料ガスＨ2 を流すようにする。When the cathode compression deformation in the cathode reducing state is completed, as shown in FIG. 1D, the oxidizing gas (air, CO 2 ) together with N 2 gas is introduced into the gas passage 5 on the cathode 2 side.
Flowing to oxidize the cathode 2 and resist N from creep deformation.
iO, and N in the gas passage 6 on the anode 3 side.
The fuel gas H 2 is caused to flow together with the two gases.
【００１４】この状態では、カソードの電解質に対する
濡れ性は再び高くなるが、カソードの空隙減少が電解質
がカソードへ戻ることを制限する。In this state, the wettability of the cathode with respect to the electrolyte becomes high again, but the void reduction of the cathode limits the return of the electrolyte to the cathode.
【００１５】上記図１（ニ）の工程が終ると、カソード
２側には酸化ガス、アノード３側には燃料ガスをそれぞ
れ供給させて通常運転を行わせるようにする。When the step of FIG. 1D is completed, the oxidizing gas is supplied to the cathode 2 side and the fuel gas is supplied to the anode 3 side to perform normal operation.
【００１６】なお、上記実施例では、一例としてセパレ
ータ４を挟んで酸化ガスと燃料ガスが並行流となるもの
について示したが、対向流となるようにしたものでもよ
く、又、ガスの給排は内部マニホールド型、外部マニホ
ールド型のいずれでもよいこと、その他本発明の要旨を
逸脱しない範囲内で種々変更を加え得ることは勿論であ
る。In the above embodiment, as an example, the oxidizing gas and the fuel gas flow in parallel with the separator 4 sandwiched between them. However, the oxidizing gas and the fuel gas may flow in opposite directions. Needless to say, may be an internal manifold type or an external manifold type, and various changes may be made without departing from the scope of the present invention.
【００１７】[0017]
【発明の効果】以上述べた如く、本発明の溶融炭酸塩型
燃料電池の再生方法によれば、カソードの素材としてＮ
ｉ粉を焼結して多孔質体としたものの酸化物であるＮｉ
Ｏを用いた溶融炭酸塩型燃料電池において、ＮｉＯは電
解質に対する濡れ性が高く、且つクリープに強いが、Ｎ
ｉは電解質に対する濡れ性が低く、且つ容易にクリープ
変形することを利用して、カソードを不活性雰囲気にし
た後、還元してＮｉＯをＮｉとし、次いで、この状態で
クリープ変形させてカソードの空隙を減少させ、カソー
ド内部に存在する電解質の余剰分を電解質板、アノード
に再配分するようにするので、電解質を外部から補給す
ることなく電解質減少に伴う電池の電圧低下を回復させ
ることができる、という優れた効果を奏し得る。As described above, according to the method for regenerating a molten carbonate fuel cell of the present invention, N is used as the cathode material.
Ni, which is an oxide of i-powder sintered into a porous body
In a molten carbonate fuel cell using O, NiO has high wettability to an electrolyte and is strong in creep, but N
i is low in wettability to an electrolyte and easily creep-deforms, so that the cathode is made an inert atmosphere, and then NiO is reduced to NiO, and then creep-deformation is performed in this state to form a void in the cathode. Is reduced and the surplus of the electrolyte present inside the cathode is redistributed to the electrolyte plate and the anode, so that the voltage drop of the battery due to the electrolyte reduction can be recovered without replenishing the electrolyte from the outside. That is, the excellent effect can be achieved.
【図１】本発明の溶融炭酸塩型燃料電池の再生方法の手
順を示すもので、（イ）は電池内部を不活性ガス雰囲気
にする工程図、（ロ）はカソード還元工程図、（ハ）は
カソード圧縮変形工程図、（ニ）はカソード酸化工程図
である。FIG. 1 shows a procedure of a method for regenerating a molten carbonate fuel cell of the present invention, in which (a) is a process diagram of making an inert gas atmosphere inside the cell, (b) is a cathode reduction process diagram, () Is a cathode compression deformation process drawing, and (D) is a cathode oxidation process drawing.
【図２】溶融炭酸塩型燃料電池スタックの一部を示す概
略図である。FIG. 2 is a schematic view showing a part of a molten carbonate fuel cell stack.
１ 電解質板 ２ カソード ３ アノード ４ セパレータ ５，６ ガス通路 1 Electrolyte Plate 2 Cathode 3 Anode 4 Separator 5,6 Gas Passage
Claims (1)
多孔質体の酸化物を用いている溶融炭酸塩型燃料電池
を、その運転温度下において、カソード側とアノード側
に不活性ガスを流して、電池内部のガスを不活性ガスに
置換させ、次に、カソード側に水素ガスを流してカソー
ドを還元し、カソードの電解質に対する濡れ性を低下さ
せ、次いで、この状態で電池全体を圧縮してカソードを
圧縮変形して、余剰となったカソード内部の電解質をカ
ソードから出して、その電解質を電解質板及びアノード
に再配分し、しかる後、カソードを酸化させることを特
徴とする溶融炭酸塩型燃料電池の再生方法。1. A molten carbonate fuel cell using a porous oxide obtained by sintering Ni powder as a material of a cathode, and an inert gas is caused to flow to the cathode side and the anode side at an operating temperature thereof. To replace the gas inside the battery with an inert gas, then flow hydrogen gas to the cathode side to reduce the cathode, reduce the wettability of the cathode to the electrolyte, and then compress the entire battery in this state. By compressing and deforming the cathode to discharge the excess electrolyte inside the cathode from the cathode, redistributing the electrolyte to the electrolyte plate and the anode, and then oxidizing the cathode. How to regenerate a fuel cell.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP5177594A JPH0714592A (en) | 1993-06-25 | 1993-06-25 | Regenerating method for molten carbonate fuel cell |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| JP5177594A JPH0714592A (en) | 1993-06-25 | 1993-06-25 | Regenerating method for molten carbonate fuel cell |
Publications (1)
| Publication Number | Publication Date |
|---|---|
| JPH0714592A true JPH0714592A (en) | 1995-01-17 |
Family
ID=16033729
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| JP5177594A Pending JPH0714592A (en) | 1993-06-25 | 1993-06-25 | Regenerating method for molten carbonate fuel cell |
Country Status (1)
| Country | Link |
|---|---|
| JP (1) | JPH0714592A (en) |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR20040002074A (en) * | 2002-06-29 | 2004-01-07 | 현대자동차주식회사 | A purging device of fuel cell system |
| KR100972188B1 (en) * | 2007-12-14 | 2010-07-26 | 한국과학기술원 | Performance recovery method of direct alcohol fuel cells |
| KR101298541B1 (en) * | 2011-12-27 | 2013-08-22 | 재단법인 포항산업과학연구원 | Method for recycling mcfc element |
| JP2018037271A (en) * | 2016-08-31 | 2018-03-08 | 東芝燃料電池システム株式会社 | Fuel cell sealing component, fuel cell, and storage method of fuel cell stack |
-
1993
- 1993-06-25 JP JP5177594A patent/JPH0714592A/en active Pending
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| KR20040002074A (en) * | 2002-06-29 | 2004-01-07 | 현대자동차주식회사 | A purging device of fuel cell system |
| KR100972188B1 (en) * | 2007-12-14 | 2010-07-26 | 한국과학기술원 | Performance recovery method of direct alcohol fuel cells |
| KR101298541B1 (en) * | 2011-12-27 | 2013-08-22 | 재단법인 포항산업과학연구원 | Method for recycling mcfc element |
| JP2018037271A (en) * | 2016-08-31 | 2018-03-08 | 東芝燃料電池システム株式会社 | Fuel cell sealing component, fuel cell, and storage method of fuel cell stack |
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