JP2007250460A - Fuel cell system - Google Patents

Fuel cell system Download PDF

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JP2007250460A
JP2007250460A JP2006075163A JP2006075163A JP2007250460A JP 2007250460 A JP2007250460 A JP 2007250460A JP 2006075163 A JP2006075163 A JP 2006075163A JP 2006075163 A JP2006075163 A JP 2006075163A JP 2007250460 A JP2007250460 A JP 2007250460A
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fuel cell
cell system
positive electrode
negative electrode
fuel
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Mitsugi Taniguchi
貢 谷口
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Mitsubishi Gas Chemical Co Inc
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    • 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

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Abstract

<P>PROBLEM TO BE SOLVED: To provide a fuel cell system for efficiently making harmless raw material organic matter and incomplete oxides, such aldehydes, ketones, carboxylic acids, carboxylic esters, and carbon monoxide, contained in emission gas constituents in the fuel cell system using organic matter as a fuel. <P>SOLUTION: The fuel cell system has an ion-conductive film 5 between a positive electrode 3 and a negative electrode 4, and has a mechanism for supplying oxidizer 1 to the positive electrode and a liquid fuel 2 containing an organic matter to the negative electrode. In the fuel cell system, entire or partial negative electrode waste matter 8 is mixed with the oxidizer and is supplied to the positive electrode. <P>COPYRIGHT: (C)2007,JPO&INPIT

Description

本発明は、正極と負極との間にイオン伝導膜を有し、正極に酸化剤を、負極に有機物含有液体燃料を供給する機構を有する燃料電池システムであって、排出ガスに含まれる未反応燃料および不完全酸化物を無害化する燃料電池システムに関する。特に直接メタノール型燃料電池から排出される未反応メタノール及び副生成物であるホルムアルデヒド、ギ酸、ギ酸メチル、一酸化炭素を無害化する燃料電池システムに関する。   The present invention is a fuel cell system having an ion conductive membrane between a positive electrode and a negative electrode, and having a mechanism for supplying an oxidant to the positive electrode and an organic substance-containing liquid fuel to the negative electrode. The present invention relates to a fuel cell system for detoxifying fuel and incomplete oxide. In particular, the present invention relates to a fuel cell system for detoxifying unreacted methanol and by-products such as formaldehyde, formic acid, methyl formate, and carbon monoxide discharged from a direct methanol fuel cell.

近年、環境対策と利便性に優れた発電システムとして燃料電池に注目が集まっている。特に燃料としてメタノール水溶液を用いる直接メタノール型燃料電池は、燃料が液体であるという特徴から、小型・携帯用として期待され、開発が進んでいる。   In recent years, attention has been focused on fuel cells as a power generation system excellent in environmental measures and convenience. In particular, a direct methanol fuel cell using a methanol aqueous solution as a fuel is expected to be small and portable because of the characteristic that the fuel is a liquid, and is being developed.

しかしながら、直接メタノール型燃料電池は燃料極での反応でメタノールの部分酸化物であるホルムアルデヒド、ギ酸、ギ酸メチル、一酸化炭素が生成してしまい、排出物中に含まれるという欠点がある。また、未反応のメタノールが排出されることもある。メタノール及びその部分酸化物は人体に有害であり、特にホルムアルデヒドは、近年シックハウス症候群の原因物質の一つとされており、厚生労働省は室内でのホルムアルデヒド濃度の基準値を０．０８ｐｐｍとしている。従って、直接メタノール型燃料電池を電源として使用するには、建物内、飛行機・電車、自動車等の交通手段など、閉空間での使用が適さないという大きな問題がある。   However, a direct methanol fuel cell has a drawback that formaldehyde, formic acid, methyl formate, and carbon monoxide, which are partial oxides of methanol, are produced by reaction at the fuel electrode and are contained in the exhaust gas. In addition, unreacted methanol may be discharged. Methanol and its partial oxides are harmful to the human body. In particular, formaldehyde is one of the causative substances of sick house syndrome in recent years. Therefore, in order to use a direct methanol fuel cell as a power source, there is a big problem that it is not suitable for use in a closed space such as in a building, an airplane / train, a vehicle or the like.

直接メタノール型燃料電池において排出物を気体と液体に分離後、気体成分を吸収または分解するフィルターを備えた気体成分回収手段を用いる方法が開示されている（例えば、特許文献１参照）。しかしながら気体成分回収手段としてフィルターを用いて吸収または分解するとの記載があるのみで、具体的に有効な手段は提示されていない。   In a direct methanol fuel cell, a method is disclosed that uses gas component recovery means that includes a filter that absorbs or decomposes gas components after separating the exhaust gas into liquid and gas (see, for example, Patent Document 1). However, there is only a description of absorption or decomposition using a filter as a gas component recovery means, and no specific effective means is presented.

一般に有害な気体成分の無害化には吸着法または分解法が用いられる。たとえばホルムアルデヒドを効率よく吸着する方法が開示されているが（例えば、特許文献２参照）、使用後吸着剤を交換するか、または吸着した成分を処理する手段が必要である。また、一酸化炭素のように活性炭やゼオライト等の一般的な吸着剤に吸着されない物質は処理されずそのまま排出される欠点がある。光触媒を用いる場合は光を当てるという操作あるいは光を当てる装置が必要となる。
特開２００３−２２３９２０号公報 特開２００１−１７９０８５号公報 Generally, an adsorption method or a decomposition method is used for detoxifying harmful gas components. For example, although a method for efficiently adsorbing formaldehyde has been disclosed (see, for example, Patent Document 2), a means for exchanging the adsorbent after use or treating the adsorbed component is required. Further, there is a disadvantage that a substance that is not adsorbed by a general adsorbent such as activated carbon or zeolite such as carbon monoxide is discharged without being treated. When a photocatalyst is used, an operation for applying light or a device for applying light is required.
JP 2003-223920 A JP 2001-179085 A

本発明の目的は、有機物を燃料とする燃料電池において排出気体成分中に含まれる原料有機物、およびアルデヒド、ケトン、カルボン酸、カルボン酸エステル、一酸化炭素等の不完全酸化物を効率良く無害化する燃料電池システムを提供することである。   The object of the present invention is to efficiently detoxify raw material organic substances contained in exhaust gas components and incomplete oxides such as aldehydes, ketones, carboxylic acids, carboxylic acid esters, and carbon monoxide in fuel cells using organic substances as fuel. To provide a fuel cell system.

本発明者は、上記の課題を解決する為に燃料電池の排出物成分を詳細に分析し鋭意検討を重ねた結果、不完全酸化物は主に負極で生成していることを見出し、負極で生じた不完全酸化物を酸化剤と共に正極に供給することによって、燃料電池性能にほとんど悪影響を与えず、コストアップに繋がる補機を燃料電池システムに設置することなく無害化できることを見出し、本発明に到達した。すなわち本発明はつぎのとおりである。
１． 正極と負極との間にイオン伝導膜を有し、正極に酸化剤を、負極に有機物含有液体燃料を供給する機構を有する燃料電池システムであって、負極排出物の全部または一部を、前記酸化剤と混合して正極に供給することを特徴とする燃料電池システム。
２． 前記イオン伝導膜がプロトン伝導性固体高分子膜である第１項記載の燃料電池システム。
３． 前記酸化剤が空気または酸素である第１項記載の燃料電池システム。
４． 前記有機物含有液体燃料がメタノールおよび水を含有する第１項記載の燃料電池システム。
５． 前記負極排出物を気体成分と液体成分に分離し、分離した液体成分を燃料として利用する第１項記載の燃料電池システム。
６． 前記正極の触媒がＰｔ担持カーボンブラックである第１項記載の燃料電池システム。
７． 前記負極の触媒がＰｔＲｕ担持カーボンブラックである第１項記載の燃料電池システム。
８． 正極と負極との間にイオン伝導膜を有し、正極に酸化剤を、負極に有機物含有液体燃料を供給する機構を有する燃料電池システムにおいて、負極排出物の全部または一部を、前記酸化剤と混合して正極に供給することを特徴とする負極排出物の無害化方法。 In order to solve the above problems, the present inventor has analyzed the exhaust cell components of the fuel cell in detail and conducted extensive studies. As a result, the inventor has found that incomplete oxide is mainly generated in the negative electrode. By supplying the generated incomplete oxide to the positive electrode together with the oxidant, it has been found that the fuel cell performance is hardly adversely affected, and it can be made harmless without installing an auxiliary machine in the fuel cell system leading to an increase in cost. Reached. That is, the present invention is as follows.
1. A fuel cell system having an ion conductive membrane between a positive electrode and a negative electrode, a mechanism for supplying an oxidizer to the positive electrode and an organic substance-containing liquid fuel to the negative electrode, wherein all or part of the negative electrode discharge A fuel cell system, wherein the fuel cell system is mixed with an oxidant and supplied to the positive electrode.
2. 2. The fuel cell system according to claim 1, wherein the ion conductive membrane is a proton conductive solid polymer membrane.
3. The fuel cell system according to claim 1, wherein the oxidant is air or oxygen.
4). The fuel cell system according to claim 1, wherein the organic substance-containing liquid fuel contains methanol and water.
5). The fuel cell system according to claim 1, wherein the negative electrode discharge is separated into a gas component and a liquid component, and the separated liquid component is used as fuel.
6). 2. The fuel cell system according to claim 1, wherein the positive electrode catalyst is Pt-supported carbon black.
7). The fuel cell system according to claim 1, wherein the negative electrode catalyst is PtRu-supported carbon black.
8). In a fuel cell system having an ion conductive membrane between a positive electrode and a negative electrode, and having a mechanism for supplying an oxidant to the positive electrode and supplying an organic substance-containing liquid fuel to the negative electrode, all or part of the negative electrode discharge is converted to the oxidant. A method for detoxifying negative electrode discharge, which is supplied to a positive electrode after being mixed with a positive electrode.

液体燃料を直接供給する燃料電池から排出される有害成分が、効率良く安定的に無害化でき、燃料電池を屋内・屋外を問わず安全に使用することができる。   The harmful components discharged from the fuel cell that directly supplies the liquid fuel can be made harmless efficiently and stably, and the fuel cell can be used safely both indoors and outdoors.

以下、メタノール水溶液を用いた直接メタノール型燃料電池からの排出物を無害化する燃料電池システムを説明するが、メタノール水溶液以外の燃料、例えば、ジメチルエーテル、ギ酸、ギ酸メチル、エタノール等を含有する燃料直接供給型燃料電池システムにも適用することができる。   Hereinafter, a fuel cell system for detoxifying emissions from a direct methanol fuel cell using an aqueous methanol solution will be described. However, a fuel directly containing a fuel other than an aqueous methanol solution such as dimethyl ether, formic acid, methyl formate, ethanol, etc. It can also be applied to a supply type fuel cell system.

直接メタノール型燃料電池用のイオン伝導膜にはプロトン伝導性固体高分子膜が用いられるが、Ｎａｆｉｏｎ（登録商標）に代表されるパーフルオロカーボンスルホン酸系高分子膜が好ましい。   A proton conductive solid polymer membrane is used as an ion conductive membrane for a direct methanol fuel cell, and a perfluorocarbon sulfonic acid polymer membrane represented by Nafion (registered trademark) is preferred.

正極および負極の触媒には、公知の触媒が用いられるが、特開２００５−６３７４９号公報に記載された方法、すなわち担体と有機塩基および還元剤の存在下、金属ハロゲン化物を液相還元し、生成した金属微粒子を担体に沈着させる方法により得られる金属担持触媒を用いることが好ましい。中でも、正極触媒にはＰｔ担持カーボンブラック、負極触媒にはＰｔＲｕ担持カーボンブラックが好適である。   As the positive electrode and negative electrode catalysts, known catalysts are used. The method described in JP-A-2005-63749, that is, a liquid halide reduction of a metal halide in the presence of a carrier, an organic base and a reducing agent, It is preferable to use a metal-supported catalyst obtained by a method of depositing the produced metal fine particles on a carrier. Among these, Pt-supported carbon black is preferable for the positive electrode catalyst, and PtRu-supported carbon black is preferable for the negative electrode catalyst.

不完全酸化物は負極から排出され、正極からはほとんど排出されない。すなわち、正極の触媒は発電環境下でクロスオーバーしてきたメタノールを二酸化炭素まで完全酸化する。このため、負極からの排出成分を正極に供給することでメタノールおよびその部分酸化物であるホルムアルデヒド、一酸化炭素、ギ酸、ギ酸メチルを酸化無害化することができる。   The incomplete oxide is discharged from the negative electrode and hardly discharged from the positive electrode. That is, the catalyst of the positive electrode completely oxidizes methanol that has crossed over to the carbon dioxide in the power generation environment. For this reason, methanol and its partial oxides, such as formaldehyde, carbon monoxide, formic acid, and methyl formate, can be oxidized and detoxified by supplying the discharge component from the negative electrode to the positive electrode.

図１に本発明の燃料電池システムの一例を示す。燃料電池の正極に空気または酸素をポンプで送り込むアクティブ型燃料電池の場合、負極からの排出成分は気液分離器において気相と液相に分離される。   FIG. 1 shows an example of a fuel cell system of the present invention. In the case of an active fuel cell in which air or oxygen is pumped to the positive electrode of the fuel cell, exhaust components from the negative electrode are separated into a gas phase and a liquid phase in a gas-liquid separator.

液相成分には未反応の燃料が含まれているため、回収して再度負極に供給してもよい。気相には二酸化炭素、未反応のメタノール、メタノールの部分酸化物であるホルムアルデヒド、一酸化炭素、ギ酸、ギ酸メチルが含まれる。この気相成分はポンプから供給される空気または酸素と混合され、正極に供給される。この際気相成分に液相成分が多少混入しても差し支えない。   Since the liquid phase component contains unreacted fuel, it may be recovered and supplied to the negative electrode again. The gas phase contains carbon dioxide, unreacted methanol, formaldehyde which is a partial oxide of methanol, carbon monoxide, formic acid, and methyl formate. This gas phase component is mixed with air or oxygen supplied from a pump and supplied to the positive electrode. At this time, the liquid phase component may be mixed to some extent in the gas phase component.

正極へ供給されるメタノール等の有機物の量はイオン伝導膜を通して正極に到達するメタノールの量より少ないため、燃料電池の出力に大きな影響はない。正極に供給されたメタノール及びその部分酸化物は正極の触媒上で酸素と反応し二酸化炭素まで完全に酸化される。正極の排出成分は未反応の空気および酸素、水、二酸化炭素である。水は気液分離器により回収し燃料の希釈に利用しても良い。   Since the amount of organic matter such as methanol supplied to the positive electrode is smaller than the amount of methanol reaching the positive electrode through the ion conductive membrane, the output of the fuel cell is not greatly affected. Methanol and its partial oxide supplied to the positive electrode react with oxygen on the positive electrode catalyst and are completely oxidized to carbon dioxide. The exhaust components of the positive electrode are unreacted air and oxygen, water, and carbon dioxide. Water may be recovered by a gas-liquid separator and used for fuel dilution.

次に本発明を、実施例をもって更に詳細に説明する。ただし、本発明はこれらに限定されるものではない。
なお、メタノールについてはメタネーターを用いＦＩＤをディテクターとしたガスクロマトグラフィー、ホルムアルデヒドについてはジニトロフェニルヒドラジンと反応させた後高速液体クロマトグラフィー、ギ酸についてはイオンクロマトグラフィーにより、それぞれ定量した。 Next, the present invention will be described in more detail with reference to examples. However, the present invention is not limited to these.
Methanol was quantified by gas chromatography using a methanator and FID as a detector, formaldehyde was reacted with dinitrophenylhydrazine and then subjected to high performance liquid chromatography, and formic acid was quantified by ion chromatography.

実施例１
イオン伝導膜として市販のＮａｆｉｏｎ（登録商標）、正極触媒として特開２００５−６３７４９号公報記載の方法により調製したＰｔ担持カーボンブラック（Ｐｔ担持量３０ｗｔ％）、負極触媒として特開２００５−６３７４９号公報記載の方法により調製したＰｔＲｕ担持カーボンブラック（Ｐｔ担持量２０ｗｔ％、Ｒｕ担持量１０ｗｔ％）を使用した電極層を有する直接メタノール型燃料電池において、図１に示すように負極排出物を気液分離し、気相成分を空気と混合して燃料電池の正極に供給した。燃料電池の運転温度は７０℃とした。正極の排出物を気液分離して気相成分および液相成分をそれぞれ分析したところ、メタノール、ギ酸、ホルムアルデヒドのいずれも基準値（メタノール：日本産業衛生学会 ２００ｐｐｍ、ホルムアルデヒド：ＷＨＯ のガイドライン値 ０．０８ｐｐｍ、ギ酸：日本産業衛生学会 ５ｐｐｍ）を大きく下回っていた。 Example 1
Commercially available Nafion (registered trademark) as an ion conductive membrane, Pt-supported carbon black prepared by the method described in JP-A-2005-63749 (Pt support amount 30 wt%) as a positive electrode catalyst, and JP-A-2005-63749 as negative electrode catalyst In a direct methanol fuel cell having an electrode layer using PtRu-supported carbon black (Pt support amount 20 wt%, Ru support amount 10 wt%) prepared by the method described above, the anode discharge is separated into gas and liquid as shown in FIG. The gas phase component was mixed with air and supplied to the positive electrode of the fuel cell. The operating temperature of the fuel cell was 70 ° C. Gas phase and liquid phase components were analyzed by gas-liquid separation of the positive electrode effluent, and methanol, formic acid, and formaldehyde were all standard values (methanol: Japan Society for Occupational Health 200 ppm, formaldehyde: WHO guideline values 0. 08 ppm, formic acid: Japan Society for Occupational Health 5 ppm).

比較例１
実施例１において負極排出物を気液分離した後、気相成分を捕集分析したところ、メタノール、ギ酸、ホルムアルデヒドのいずれも基準値（メタノール：日本産業衛生学会 ２００ｐｐｍ、ホルムアルデヒド：ＷＨＯ のガイドライン値 ０．０８ｐｐｍ、ギ酸：日本産業衛生学会 ５ｐｐｍ）を大きく上回っていた。 Comparative Example 1
After gas-liquid separation of the anode discharge in Example 1, gas phase components were collected and analyzed. As a result, methanol, formic acid, and formaldehyde were all standard values (methanol: Japanese Industrial Hygiene Society 200 ppm, formaldehyde: WHO guideline value 0 .08 ppm, formic acid: Japan Society for Occupational Health 5 ppm).

燃料電池システムの一例An example of a fuel cell system

符号の説明Explanation of symbols

１ 空気または酸素
２ 有機物燃料
３ 正極
４ 負極
５ イオン伝導膜
６ 燃料電池
７ 正極排出物
８ 負極排出物
９ 気液分離器
１０ 気相成分
１１ 液相成分
DESCRIPTION OF SYMBOLS 1 Air or oxygen 2 Organic fuel 3 Positive electrode 4 Negative electrode 5 Ion conduction membrane 6 Fuel cell 7 Positive electrode discharge 8 Negative electrode discharge 9 Gas-liquid separator 10 Gas phase component 11 Liquid phase component

Claims (8)

正極と負極との間にイオン伝導膜を有し、正極に酸化剤を、負極に有機物含有液体燃料を供給する機構を有する燃料電池システムであって、負極排出物の全部または一部を、前記酸化剤と混合して正極に供給することを特徴とする燃料電池システム。   A fuel cell system having an ion conductive membrane between a positive electrode and a negative electrode, a mechanism for supplying an oxidant to the positive electrode and an organic substance-containing liquid fuel to the negative electrode, wherein all or part of the negative electrode discharge A fuel cell system, wherein the fuel cell system is mixed with an oxidant and supplied to the positive electrode. 前記イオン伝導膜がプロトン伝導性固体高分子膜である請求項１記載の燃料電池システム。   The fuel cell system according to claim 1, wherein the ion conductive membrane is a proton conductive solid polymer membrane. 前記酸化剤が空気または酸素である請求項１記載の燃料電池システム。   The fuel cell system according to claim 1, wherein the oxidant is air or oxygen. 前記有機物含有液体燃料がメタノールおよび水を含有する請求項１記載の燃料電池システム。   The fuel cell system according to claim 1, wherein the organic substance-containing liquid fuel contains methanol and water. 前記負極排出物を気体成分と液体成分に分離し、分離した液体成分を燃料として利用する請求項１記載の燃料電池システム。   The fuel cell system according to claim 1, wherein the negative electrode discharge is separated into a gas component and a liquid component, and the separated liquid component is used as fuel. 前記正極の触媒がＰｔ担持カーボンブラックである請求項１記載の燃料電池システム。   2. The fuel cell system according to claim 1, wherein the positive electrode catalyst is Pt-supported carbon black. 前記負極の触媒がＰｔＲｕ担持カーボンブラックである請求項１記載の燃料電池システム。   2. The fuel cell system according to claim 1, wherein the negative electrode catalyst is PtRu-supported carbon black. 正極と負極との間にイオン伝導膜を有し、正極に酸化剤を、負極に有機物含有液体燃料を供給する機構を有する燃料電池システムにおいて、負極排出物の全部または一部を、前記酸化剤と混合して正極に供給することを特徴とする負極排出物の無害化方法。   In a fuel cell system having an ion conductive membrane between a positive electrode and a negative electrode, and having a mechanism for supplying an oxidant to the positive electrode and supplying an organic substance-containing liquid fuel to the negative electrode, all or part of the negative electrode discharge is converted to the oxidant. A method for detoxifying negative electrode discharge, which is supplied to the positive electrode after being mixed with the positive electrode.
JP2006075163A 2006-03-17 2006-03-17 Fuel cell system Pending JP2007250460A (en)

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013247114A (en) * 2012-05-29 2013-12-09 Commissariat A L'energie Atomique Et Aux Energies Alternatives Method for measuring reproducibility of n unitary ion exchange membrane/electrode assemblies using pollutant delivery

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013247114A (en) * 2012-05-29 2013-12-09 Commissariat A L'energie Atomique Et Aux Energies Alternatives Method for measuring reproducibility of n unitary ion exchange membrane/electrode assemblies using pollutant delivery

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