JP2007153667A - Hydrogen generator and fuel cell - Google Patents

Hydrogen generator and fuel cell Download PDF

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JP2007153667A
JP2007153667A JP2005350897A JP2005350897A JP2007153667A JP 2007153667 A JP2007153667 A JP 2007153667A JP 2005350897 A JP2005350897 A JP 2005350897A JP 2005350897 A JP2005350897 A JP 2005350897A JP 2007153667 A JP2007153667 A JP 2007153667A
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hydrogen
water
aluminum
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hydrogen generator
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JP5156974B2 (en
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Gitaku Kin
義澤 金
Tokichi Ichige
東吉 市毛
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SAISEIKO KK
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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
    • Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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Abstract

<P>PROBLEM TO BE SOLVED: To provide a hydrogen gas generator in which raw materials are inexpensive and a production process is simple, and to configure a fuel cell using generated hydrogen as fuel. <P>SOLUTION: The hydrogen generator comprises a reacting substance prepared by mixing calcium oxide and/or magnesium oxide with at least ≥1% of aluminum and a water permeable container containing the reacting substance, wherein hydrogen is generated by immersing the water permeable container in water. The water permeable container is a bag-like container made of a nonwoven fabric or cotton cloth. The calcium oxide is obtained by firing limestone, calcite, aragonite or stalactite at 1,000-1,200°C and pulverizing it. The aluminum is obtained by reducing a metal aluminum ingot or an aluminum product to powder. <P>COPYRIGHT: (C)2007,JPO&INPIT

Description

本発明は、効率良く水素ガスを発生させる水素ガスの発生具に関する。また、発生させた水素を燃料とする燃料電池に関する。   The present invention relates to a hydrogen gas generator that efficiently generates hydrogen gas. The present invention also relates to a fuel cell using generated hydrogen as fuel.

水素の製造方法は、水蒸気改質法、部分酸化法、副生ガス利用、水電解の方法等がある。一例として、原料にナフサ軽質油、天然ガス、石油精製オフガス（プロパン、ブタン等）の炭化水素を原料とする水蒸気改質法においては、原料を７００〜８５０℃で、ＮｉＯ触媒で水蒸気ガスと反応させ、ＣＯ、ＣＯ２、Ｈ２の混合物である合成ガスを発生させ、分離生成するものである。反応式は、ＣｍＨｎ＋ｍＨ２Ｏ＝ｍＣＯ＋（ｍ＋ｎ／２）Ｈ２で示される。また、光エネルギーを用いて水を水素と酸素に分解する方法においては、陽極にｎ型半導体のＴｉＯ２、陰極にＰｔを用い、両極を結んで半導体電極に太陽光を照射すると電解質溶液の水が電気分解され、Ｐｔ電極から水素発生するものである。反応式は、２Ｈ２Ｏ＝Ｏ２＋４ｅ−＋４Ｈ＋：２Ｈ＋＋２ｅ−＝Ｈ２で示される。
また、特開２００５−６７９７０号公報には、有機造岩鉱物を焼成した水素発生材が記載されている。そして、有機造岩鉱物は、原石の状態でケイ素（Ｓｉ）、アルミニウム（Ａｌ）、鉄（Ｆｅ）、チタン（Ｔｉ）、カルシウム（Ｃａ）、マグネシウム（Ｍｇ）、カリウム（Ｋ）、ナトリウム（Ｎａ）、ロジウム（Ｒｈ）、ジルコニウム（Ｚｒ）、ルビジウム（Ｒｂ）、ストロンチウム（Ｓｒ）、亜鉛（Ｚｎ）、銅（Ｃｕ）、ニッケル（Ｎｉ）、マンガン（Ｍｎ）、塩素（Ｃｌ）、硫黄（Ｓ）、燐（Ｐ）、モリブデン（Ｍｏ）、炭素（Ｃ）などで組成されている。明細書中には、水と接触させるだけで、水素ガスの製造が簡単且つ低コストに行えることが記載されている。しかし、発生する水素ガスは極めて微量であるから、水素ガスの供給手段として実用的でない。一方、実用レベルでは、上述したような水の電気分解や炭化水素を原料とする製造方法等があるが、設備コストや製造コストが高い。
特開２００５−６７９７０号公報 Examples of the method for producing hydrogen include a steam reforming method, a partial oxidation method, use of by-product gas, and a water electrolysis method. As an example, in a steam reforming method using naphtha light oil, natural gas, and petroleum refined offgas (propane, butane, etc.) as raw materials as raw materials, the raw materials are reacted with steam gas at 700 to 850 ° C. with NiO catalyst. To generate a synthesis gas that is a mixture of CO, CO 2 , and H 2 , and separate and generate it. The reaction formula is represented by CmHn + mH 2 O = mCO + (m + n / 2) H 2 . Also, in the method of decomposing water into hydrogen and oxygen using light energy, the n-type semiconductor TiO 2 is used for the anode, Pt is used for the cathode, and both electrodes are connected to irradiate the semiconductor electrode with sunlight. Is electrolyzed to generate hydrogen from the Pt electrode. The reaction formula is represented by 2H 2 O═O 2 + 4e − + 4H + : 2H + + 2e − = H 2 .
Japanese Patent Laid-Open No. 2005-67970 describes a hydrogen generating material obtained by firing an organic rock-forming mineral. Organic rock-forming minerals are in the form of raw stones such as silicon (Si), aluminum (Al), iron (Fe), titanium (Ti), calcium (Ca), magnesium (Mg), potassium (K), sodium (Na ), Rhodium (Rh), zirconium (Zr), rubidium (Rb), strontium (Sr), zinc (Zn), copper (Cu), nickel (Ni), manganese (Mn), chlorine (Cl), sulfur (S ), Phosphorus (P), molybdenum (Mo), carbon (C), and the like. In the specification, it is described that hydrogen gas can be produced easily and at low cost simply by contacting with water. However, since the generated hydrogen gas is extremely small, it is not practical as a hydrogen gas supply means. On the other hand, on the practical level, there are the above-described electrolysis of water and a production method using hydrocarbon as a raw material, but the equipment cost and production cost are high.
JP 2005-67970 A

本発明は上述した問題点に鑑み、原料が安く、生産プロセスが簡単な水素ガスの発生具を提供することであり、また、発生させた水素を燃料として燃料電池を構成することである。   In view of the above-described problems, the present invention is to provide a hydrogen gas generator having a low cost raw material and a simple production process, and to constitute a fuel cell using the generated hydrogen as a fuel.

上記目的を達成するため、本発明の水素発生具は、酸化カルシウムおよび／または酸化マグネシウムに、少なくともアルミニウムを１％以上混合させた反応物質と、該反応物質を収納する透水性容器とを備えており、前記透水性容器を水に漬けることにより水素を発生させるようにしたことを特徴とする。また、前記透水性容器は、不織布もしくは綿布で形成した袋状容器であることを特徴とする。前記酸化カルシウムは、石灰石、方解石、アラゴナイト、鍾乳石を１０００℃から１２００℃で焼き、粉砕したものであることを特徴とする。前記アルミニウムは、金属アルミニウムインゴットもしくはアルミニウム製品を粉末状にしたものであることを特徴とする。
また、本発明の燃料電池は、請求項１ないし４に記載の水素発生具で発生させた気体を燃料とする。 In order to achieve the above object, a hydrogen generator according to the present invention includes a reactant obtained by mixing at least 1% of aluminum with calcium oxide and / or magnesium oxide, and a water permeable container for containing the reactant. In addition, hydrogen is generated by immersing the water-permeable container in water. The water-permeable container is a bag-shaped container formed of a nonwoven fabric or cotton cloth. The calcium oxide is obtained by baking and pulverizing limestone, calcite, aragonite, and stalactite at 1000 to 1200 ° C. The aluminum is a metal aluminum ingot or a powdered aluminum product.
Moreover, the fuel cell of this invention uses the gas generated with the hydrogen generator of Claims 1 thru | or 4 as a fuel.

本発明の水素発生具は、水が利用できる環境で容易に水素を発生させることができる。また、水素ボンベ等の必要がなく、安全に運搬することができる。透水性容器としての不織布や綿布は水を好適に浸透させ、且つ、粉末状の反応物質を収納することできる。反応物質の原料は、石灰石、方解石、アラゴナイト、鍾乳石等の鉱石を粉砕し、また、金属アルミニウムインゴットやアルミニウム製品を粉末状にして混合することにより、安価なものとすることができる。
請求項１ないし４に記載の水素発生具で発生させた気体は、水蒸気を含み、これを燃料とすることにより、効率の良い燃料電池とすることができる。 The hydrogen generator of the present invention can easily generate hydrogen in an environment where water is available. Further, there is no need for a hydrogen cylinder or the like, and it can be safely transported. Nonwoven fabrics and cotton fabrics as water permeable containers can suitably permeate water and contain a reactive substance in powder form. The reactant material can be made inexpensive by grinding ores such as limestone, calcite, aragonite, and stalactite, and by mixing a metal aluminum ingot or aluminum product in powder form.
The gas generated by the hydrogen generator according to any one of claims 1 to 4 contains water vapor, and by using this as fuel, an efficient fuel cell can be obtained.

図１（ａ）は、本発明の水素発生具１０を示す斜視図であり、図１（ｂ）は、図１（ａ）におけるＡ−Ａ線断面図である。この図１（ａ）、図１（ｂ）に示すように、水素発生具１０は、袋状の透水性容器３の中に、水と反応して水素を発生する反応物質１を収納したものである。反応物質１は、酸化カルシウムおよび／または酸化マグネシウムに、少なくともアルミニウムを１％以上混合させたものである。因みに、酸化カルシウム（生石灰）は、天然の石灰石、方解石、アラゴナイト、鍾乳石等の鉱石を１０００℃〜１２００℃の高温で焼き、粉砕し製造される。酸化マグネシウムは、天然にあるマグネサイト及びマグネサイト鉱物を含む鉱石を１０００℃〜１２００℃の高温で焼き粉砕されたものである。また、アルミニウムは、工業用金属アルミニウムインゴットあるいはアルミニウム製品を粉末状にして製造される。   Fig.1 (a) is a perspective view which shows the hydrogen generator 10 of this invention, FIG.1 (b) is the sectional view on the AA line in Fig.1 (a). As shown in FIGS. 1 (a) and 1 (b), the hydrogen generator 10 is a bag-shaped water permeable container 3 that contains a reactant 1 that generates hydrogen by reacting with water. It is. The reactant 1 is a mixture of calcium oxide and / or magnesium oxide mixed with at least 1% aluminum. Incidentally, calcium oxide (quick lime) is produced by baking or crushing ores such as natural limestone, calcite, aragonite, and stalactite at a high temperature of 1000 ° C to 1200 ° C. Magnesium oxide is obtained by baking and crushing ores containing natural magnesite and magnesite mineral at a high temperature of 1000 ° C to 1200 ° C. Aluminum is produced by powdering an industrial metal aluminum ingot or aluminum product.

透水性容器３は、水がよく浸透し、発生した水素ガスが漏れるような不織布や綿布等で袋状に製造される。因みに、不織布は、繊維の集積層を形成するとともに、繊維同士を結合させたものであり、水が浸透し通気性を有する。原料は、ポリエステルなどの合成繊維が多く使われるが、天然繊維、合成繊維を始めガラス・金属・セラミックス・パルプ・炭素繊維などで製造されることもある。しかし、このような不織布に限定されることはなく、例えば、通水口と発生した水素が通過できるような通気口とを設けたプラスチック製容器として、透水性容器３を構成することもできる。このような透水性容器３の中に、上述した反応物質１を収納し、通水口から水を通水させるとともに、発生した水素を通気口から収集するようにする。   The water permeable container 3 is manufactured in a bag shape with a nonwoven fabric or cotton cloth that allows water to permeate well and the generated hydrogen gas leaks. Incidentally, the non-woven fabric forms a fiber accumulation layer and bonds the fibers to each other, and water penetrates and has air permeability. Synthetic fibers such as polyester are often used as raw materials, but natural fibers and synthetic fibers as well as glass, metal, ceramics, pulp, and carbon fibers are sometimes used. However, it is not limited to such a nonwoven fabric, For example, the water-permeable container 3 can also be comprised as a plastic container provided with the water vent and the vent hole through which the generated hydrogen can pass. In such a water permeable container 3, the above-described reactant 1 is accommodated to allow water to flow from the water passage and to collect generated hydrogen from the vent.

綿布縫製袋（透水性容器３）の中に、酸化カルシウム（ＣａＯ）４７．２５７ｇと、酸化マグネシウム（ＭｇＯ）２０．２５３ｇと、アルミニウム（Ａｌ）３２．４９ｇを均一に混合するとともに、２００メッシュに粉砕して粉末とした反応物質１（トータル１００ｇ）を入れて水素発生具１０とした。この水素発生具１０を、水を入れた容器４の中に沈めたところ、気泡が発生した（図２参照）。この気泡の発生は、水素発生具１０を水の底に沈めた直後から発生し、綿布縫製袋が濡れることにより、さらに勢いがよくなり、１０分程度続いた。この気体を試験管に集め着火したところ爆発的に発火し、試験管口部に水滴が付着した。このことから、発生した気体は水素であることが確認された。尚、発生した気体をガス収集具６で収集したところ、４１．４Ｌであった。発生した気体の内、水温飽和水蒸気１．６８％を除くと純粋な水素は４０．７Ｌと考えられる。因みに、本実施例による水素ガスの発生は、以下のような反応式で表すことができる。
２ＣａＯ＋２Ａｌ＋３Ｈ２Ｏ＝Ｃａ２Ａｌ２Ｏ５＋３Ｈ２
２ＭｇＯ＋２Ａｌ＋３Ｈ２Ｏ＝Ｍｇ２Ａｌ２Ｏ５＋３Ｈ２ In a cotton cloth sewing bag (water-permeable container 3), 47.257 g of calcium oxide (CaO), 20.253 g of magnesium oxide (MgO), and 32.49 g of aluminum (Al) are uniformly mixed, and 200 mesh Reactive material 1 (total 100 g) that was pulverized into powder was put into hydrogen generator 10. When the hydrogen generator 10 was submerged in the container 4 containing water, bubbles were generated (see FIG. 2). The generation of the bubbles occurred immediately after the hydrogen generator 10 was submerged in the bottom of the water, and the momentum was further improved by the wetness of the cotton cloth sewing bag, which lasted for about 10 minutes. When this gas was collected in a test tube and ignited, it ignited explosively and water droplets adhered to the test tube opening. From this, it was confirmed that the generated gas was hydrogen. The generated gas was collected by the gas collector 6 and found to be 41.4 L. In the generated gas, pure hydrogen is considered to be 40.7 L excluding 1.68% water temperature saturated water vapor. Incidentally, the generation of hydrogen gas according to the present embodiment can be expressed by the following reaction formula.
2CaO + 2Al + 3H 2 O = Ca 2 Al 2 O 5 + 3H 2
2MgO + 2Al + 3H 2 O = Mg 2 Al 2 O 5 + 3H 2

本発明の水素発生具１０は、水素の発生源を、容易に持ち運びできるようにしたことにより、水素を運搬する際に伴うリスクが回避できる。また、上記した反応は発熱反応であり、副産物として熱水が得られるので、例えば、家庭内における熱源として熱水が利用可能となる。このことから、家庭内で、直接的に水素を発電や燃料とした場合と、水素の発生源として水素発生具１０を利用した場合とを比較すると、凡そ、水素を利用することによるエネルギー効率が３５％程度から８０％程度に向上する。   The hydrogen generator 10 of the present invention can easily carry a hydrogen generation source, thereby avoiding the risk associated with transporting hydrogen. Moreover, since the above-described reaction is an exothermic reaction and hot water is obtained as a by-product, for example, hot water can be used as a heat source in the home. From this, comparing the case where hydrogen is directly used for power generation or fuel in the home and the case where the hydrogen generator 10 is used as a hydrogen generation source, the energy efficiency of using hydrogen is almost equal. It improves from about 35% to about 80%.

図３は、発生させた水素が発電に利用できる燃料電池８を模式的に示したものである。本発明の水素発生具１０で発生させた水素は、電極を介して電解質（ＫＯＨ）に溶解するが、陰極側でイオン化するので電子を放出する。水素イオンは、陽極側で電子を受け取った酸素分子と結合し水となる。このような燃料電池は、水素の供給により発電できる。また、本発明の水素発生具１０は、水道水、河湖水、海水等、如何なる水でも利用できる。このことから、本発明の水素発生具１０は、給電設備のない場所でも、水が在れば発電できる発電機を構成することができる。そして、生じる化合物や水は、天然のものであり、また、既存の化石燃料を使用しないのであるから、環境を汚染することがない。   FIG. 3 schematically shows a fuel cell 8 in which the generated hydrogen can be used for power generation. The hydrogen generated by the hydrogen generator 10 of the present invention is dissolved in the electrolyte (KOH) through the electrode, but is ionized on the cathode side, so that electrons are emitted. Hydrogen ions combine with oxygen molecules that have received electrons on the anode side to become water. Such a fuel cell can generate electricity by supplying hydrogen. In addition, the hydrogen generator 10 of the present invention can be used with any water such as tap water, river lake water, seawater and the like. From this, the hydrogen generator 10 of the present invention can constitute a generator that can generate power if water is present even in a place where there is no power supply facility. The resulting compounds and water are natural and do not use existing fossil fuels, so they do not pollute the environment.

尚、本発明の水素発生具１０で発生させた気体は水素が９８〜９９％であるが、１〜２％の水蒸気を含む。このような気体は、水素の他に水蒸気を含むことから、水素分子が電極を介して電解質（ＫＯＨ）に溶解し易くなるので、燃料電池８の燃料として好適である。   In addition, although the gas generated with the hydrogen generator 10 of the present invention is 98 to 99% of hydrogen, it contains 1 to 2% of water vapor. Since such a gas contains water vapor in addition to hydrogen, hydrogen molecules are easily dissolved in the electrolyte (KOH) through the electrode, and thus is suitable as a fuel for the fuel cell 8.

高圧水素もしくは液体水素の運搬には、これらを収納するための貯蔵缶や、運送設備に高度な技術を要する。したがって、水素を原料とする燃料電池の普及には、水素を直接運搬するより、むしろ、水素を発生させる原料を運搬するようにするほうが有利である。本発明は、水素を発生させる原料が安価に供給できるものであり、水素を必要とする如何なる場所にでも手軽に運べるので、水素の運搬に利便性を提供できるものである。
さらに、本発明の水素発生具１０は、河川や湖沼の汚濁を清浄化する浄化材としても利用できる。水素発生具１０は水素を発生することにより、マイナスイオン化して浮遊している有機物等からマイナスイオンを奪い、懸濁状態の有機物を凝集させ沈降を促進する働きを有する。 In order to transport high-pressure hydrogen or liquid hydrogen, advanced technology is required for storage canisters for storing them and transportation facilities. Therefore, for the spread of fuel cells using hydrogen as a raw material, it is more advantageous to transport a raw material that generates hydrogen rather than directly transporting hydrogen. According to the present invention, a raw material for generating hydrogen can be supplied at a low cost, and can be easily transported to any place where hydrogen is required. Therefore, convenience for transporting hydrogen can be provided.
Furthermore, the hydrogen generator 10 of the present invention can also be used as a purification material for purifying the pollution of rivers and lakes. The hydrogen generator 10 has a function of generating negative ions to remove negative ions from the floating organic substances and the like, thereby aggregating suspended organic substances and promoting sedimentation.

（ａ）は、本発明の水素発生具を示す斜視図であり、（ｂ）は、（ａ）におけるＡ−Ａ線断面図である。(A) is a perspective view which shows the hydrogen generator of this invention, (b) is the sectional view on the AA line in (a). 水素の発生を示す説明図である。It is explanatory drawing which shows generation | occurrence | production of hydrogen. 発生させた水素の利用形態を示した説明図である。It is explanatory drawing which showed the utilization form of the produced | generated hydrogen.

符号の説明Explanation of symbols

１ 反応物質
３ 透水性容器
４ 容器
６ ガス収集具
８ 燃料電池
１０ 水素発生具 DESCRIPTION OF SYMBOLS 1 Reactive substance 3 Water-permeable container 4 Container 6 Gas collection tool 8 Fuel cell 10 Hydrogen generator

Claims (5)

酸化カルシウムおよび／または酸化マグネシウムに、少なくともアルミニウムを１％以上混合させた反応物質と、該反応物質を収納する透水性容器とを備えており、前記透水性容器を水に漬けることにより水素を発生させるようにしたことを特徴とする水素発生具。   It has a reaction material in which at least 1% of aluminum is mixed with calcium oxide and / or magnesium oxide, and a water permeable container containing the reaction material. Hydrogen is generated by immersing the water permeable container in water. A hydrogen generator characterized by being made to cause. 前記透水性容器は、不織布もしくは綿布で形成した袋状容器あることを特徴とする水素発生具。   The hydrogen permeable tool is characterized in that the water permeable container is a bag-shaped container formed of a nonwoven fabric or a cotton cloth. 前記酸化カルシウムは、石灰石、方解石、アラゴナイト、鍾乳石を１０００℃から１２００℃で焼き、粉砕したものであることを特徴とする水素発生具。   The hydrogen generator is characterized in that the calcium oxide is obtained by baking and pulverizing limestone, calcite, aragonite, and stalactite at 1000 to 1200 ° C. 前記アルミニウムは、金属アルミニウムインゴットもしくはアルミニウム製品を粉末状にしたものであることを特徴とする水素発生具。   The aluminum generator is a metal aluminum ingot or a powdered aluminum product. 請求項１ないし４に記載の水素発生具で発生させた気体を燃料とすることを特徴とする燃料電池。   5. A fuel cell, wherein the gas generated by the hydrogen generator according to claim 1 is used as fuel.
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