JP2002356301A - Production method for hydrogen and its apparatus - Google Patents
Production method for hydrogen and its apparatusInfo
- Publication number
- JP2002356301A JP2002356301A JP2001168418A JP2001168418A JP2002356301A JP 2002356301 A JP2002356301 A JP 2002356301A JP 2001168418 A JP2001168418 A JP 2001168418A JP 2001168418 A JP2001168418 A JP 2001168418A JP 2002356301 A JP2002356301 A JP 2002356301A
- Authority
- JP
- Japan
- Prior art keywords
- electrode
- working electrode
- hydrogen
- film
- light
- 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
- 239000001257 hydrogen Substances 0.000 title claims abstract description 66
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 66
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims abstract description 64
- 238000004519 manufacturing process Methods 0.000 title claims 4
- 239000011941 photocatalyst Substances 0.000 claims abstract description 28
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 27
- 230000001699 photocatalysis Effects 0.000 claims abstract description 26
- 238000006243 chemical reaction Methods 0.000 claims abstract description 8
- 238000000034 method Methods 0.000 claims description 16
- 239000008151 electrolyte solution Substances 0.000 claims description 11
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 9
- 238000004768 lowest unoccupied molecular orbital Methods 0.000 claims description 9
- 230000001678 irradiating effect Effects 0.000 claims description 7
- 229910052751 metal Inorganic materials 0.000 claims description 6
- 239000002184 metal Substances 0.000 claims description 6
- 239000002904 solvent Substances 0.000 claims description 6
- 239000007772 electrode material Substances 0.000 claims description 5
- 230000001747 exhibiting effect Effects 0.000 claims description 4
- -1 bipyridine metal complex Chemical class 0.000 claims description 3
- 238000006555 catalytic reaction Methods 0.000 claims description 3
- 150000002431 hydrogen Chemical class 0.000 claims description 3
- IEQIEDJGQAUEQZ-UHFFFAOYSA-N phthalocyanine Chemical compound N1C(N=C2C3=CC=CC=C3C(N=C3C4=CC=CC=C4C(=N4)N3)=N2)=C(C=CC=C2)C2=C1N=C1C2=CC=CC=C2C4=N1 IEQIEDJGQAUEQZ-UHFFFAOYSA-N 0.000 claims description 3
- 150000004032 porphyrins Chemical class 0.000 claims description 3
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 abstract description 22
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 abstract description 11
- 239000004408 titanium dioxide Substances 0.000 abstract description 10
- 239000011521 glass Substances 0.000 abstract description 8
- 239000000758 substrate Substances 0.000 abstract description 8
- 239000012327 Ruthenium complex Substances 0.000 abstract description 6
- 229910052697 platinum Inorganic materials 0.000 abstract description 6
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 abstract description 6
- 229910052721 tungsten Inorganic materials 0.000 abstract description 6
- 239000010937 tungsten Substances 0.000 abstract description 6
- 238000010521 absorption reaction Methods 0.000 abstract 1
- RHZWSUVWRRXEJF-UHFFFAOYSA-N indium tin Chemical compound [In].[Sn] RHZWSUVWRRXEJF-UHFFFAOYSA-N 0.000 abstract 1
- 239000000049 pigment Substances 0.000 abstract 1
- 238000002791 soaking Methods 0.000 abstract 1
- 229910001887 tin oxide Inorganic materials 0.000 abstract 1
- 239000010408 film Substances 0.000 description 41
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 10
- 239000001301 oxygen Substances 0.000 description 10
- 229910052760 oxygen Inorganic materials 0.000 description 10
- 235000010215 titanium dioxide Nutrition 0.000 description 10
- 239000010409 thin film Substances 0.000 description 9
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 6
- 239000007789 gas Substances 0.000 description 5
- 230000003647 oxidation Effects 0.000 description 4
- 238000007254 oxidation reaction Methods 0.000 description 4
- 229910002092 carbon dioxide Inorganic materials 0.000 description 3
- 239000001569 carbon dioxide Substances 0.000 description 3
- 238000010304 firing Methods 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 2
- 239000003054 catalyst Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000005868 electrolysis reaction Methods 0.000 description 2
- 239000000446 fuel Substances 0.000 description 2
- 238000004817 gas chromatography Methods 0.000 description 2
- 241000255777 Lepidoptera Species 0.000 description 1
- XHCLAFWTIXFWPH-UHFFFAOYSA-N [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] Chemical compound [O-2].[O-2].[O-2].[O-2].[O-2].[V+5].[V+5] XHCLAFWTIXFWPH-UHFFFAOYSA-N 0.000 description 1
- 230000004913 activation Effects 0.000 description 1
- 125000004429 atom Chemical group 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000003411 electrode reaction Methods 0.000 description 1
- 239000002737 fuel gas Substances 0.000 description 1
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 description 1
- WABPQHHGFIMREM-UHFFFAOYSA-N lead(0) Chemical compound [Pb] WABPQHHGFIMREM-UHFFFAOYSA-N 0.000 description 1
- 239000000463 material Substances 0.000 description 1
- QGLKJKCYBOYXKC-UHFFFAOYSA-N nonaoxidotritungsten Chemical compound O=[W]1(=O)O[W](=O)(=O)O[W](=O)(=O)O1 QGLKJKCYBOYXKC-UHFFFAOYSA-N 0.000 description 1
- SOQBVABWOPYFQZ-UHFFFAOYSA-N oxygen(2-);titanium(4+) Chemical class [O-2].[O-2].[Ti+4] SOQBVABWOPYFQZ-UHFFFAOYSA-N 0.000 description 1
- 239000002245 particle Substances 0.000 description 1
- 238000007146 photocatalysis Methods 0.000 description 1
- 150000003057 platinum Chemical class 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 230000006798 recombination Effects 0.000 description 1
- 238000005215 recombination Methods 0.000 description 1
- 239000000243 solution Substances 0.000 description 1
- 238000004528 spin coating Methods 0.000 description 1
- 229910001930 tungsten oxide Inorganic materials 0.000 description 1
- 238000001771 vacuum deposition Methods 0.000 description 1
- 229910001935 vanadium oxide Inorganic materials 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
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
- Y02E60/36—Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
Landscapes
- Catalysts (AREA)
- Electrodes For Compound Or Non-Metal Manufacture (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Abstract
Description
【０００１】[0001]
【発明の属する技術分野】本発明は、水或いはアルコー
ルもしくはこれらを溶媒とする電解質溶液のいずれかか
ら水素を生成する方法とその装置に関する。BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method and an apparatus for producing hydrogen from either water or alcohol or an electrolyte solution using these as a solvent.
【０００２】[0002]
【従来の技術】近年になり、光触媒がこうした水素生成
に用いられつつあり、種々の技術が提案されている。例
えば、特開平１１−２４６９８５号公報では、光触媒か
らなる光電極と白金電極とをリード線で導通し、光電極
に光照射する技術が提案されている。2. Description of the Related Art In recent years, photocatalysts have been used for such hydrogen generation, and various techniques have been proposed. For example, Japanese Patent Application Laid-Open No. H11-246985 proposes a technique in which a photoelectrode made of a photocatalyst and a platinum electrode are electrically connected by a lead wire, and light is irradiated to the photoelectrode.
【０００３】[0003]
【発明が解決しようとする課題】上記公報で提案された
水素生成手法によれば、それまでのものに比べて水素生
成効率の向上をもたらすことができるものの、更なる効
率向上が求められている。According to the hydrogen generation method proposed in the above publication, although the hydrogen generation efficiency can be improved as compared with the prior art, further improvement in efficiency is required. .
【０００４】本発明は、上記問題点を解決するためにな
され、水素生成の効率向上を図ることを目的とする。The present invention has been made to solve the above problems, and has as its object to improve the efficiency of hydrogen generation.
【０００５】[0005]
【課題を解決するための手段およびその作用・効果】か
かる課題の少なくとも一部を解決するため、本発明の水
素生成方法は、水或いはアルコールもしくはこれらを溶
媒とする電解質溶液のいずれかから水素を生成する方法
であって、光の照射を受けると正孔と電子を生成する光
触媒活性を呈する光触媒の膜が電極膜として形成された
第１作用極と、電極触媒作用を果たす電極材料の膜が電
極膜として形成された第２作用極とを、前記水或いは前
記電解質溶液中に浸漬された状態とする工程Ａと、前記
第１作用極の電極膜に、前記光触媒活性の励起可能な光
を照射すると共に、前記第１と第２の作用極の電極膜間
に、前記第１作用極の側をプラス側にして直流電圧を印
加する工程Ｂとを備え、前記第２作用極の電極膜で水素
を生成することを特徴とする。Means for Solving the Problems and Action / Effect thereof To solve at least a part of the problems, the hydrogen generation method of the present invention converts hydrogen from either water or alcohol or an electrolyte solution using these as a solvent. A first working electrode in which a photocatalytic film exhibiting photocatalytic activity for generating holes and electrons when irradiated with light is formed as an electrode film, and a film of an electrode material performing an electrocatalytic action is formed. A step A of bringing the second working electrode formed as an electrode film into a state of being immersed in the water or the electrolyte solution; and applying the light capable of exciting the photocatalytic activity to the electrode film of the first working electrode. Irradiating and applying a DC voltage between the electrode films of the first and second working electrodes with the side of the first working electrode being a plus side, comprising the steps of: To produce hydrogen with And butterflies.
【０００６】また、上記課題の少なくとも一部を解決す
るため、本発明の水素生成装置は、水或いはアルコール
もしくはこれらを溶媒とする電解質溶液のいずれかから
水素を生成する装置であって、光の照射を受けると正孔
と電子を生成する光触媒活性を呈する光触媒の膜が電極
膜として形成された第１作用極と、電極触媒作用を果た
す電極材料の膜が電極膜として形成された第２作用極と
を、前記水或いは前記電解質溶液中に浸漬された状態で
備える電極反応槽と、前記第１作用極の電極膜に、前記
光触媒活性の励起可能な光を照射する光照射手段と、該
光照射手段による光照射の実行の間に、前記第１と第２
の作用極の電極膜間に、前記第１作用極の側をプラス側
にして直流電圧を印加する電圧印加手段とを備え、前記
第２作用極の電極膜で水素を生成することを特徴とす
る。Further, in order to solve at least a part of the above-mentioned problems, a hydrogen generator of the present invention is an apparatus for generating hydrogen from water, alcohol or an electrolyte solution using these as a solvent. A first working electrode in which a photocatalytic film exhibiting photocatalytic activity that generates holes and electrons when irradiated is formed as an electrode film, and a second working electrode in which a film of an electrode material that performs electrode catalysis is formed as an electrode film. An electrode reaction tank having the electrode in a state of being immersed in the water or the electrolyte solution; and a light irradiation unit for irradiating the electrode film of the first working electrode with light capable of exciting the photocatalytic activity. During the execution of light irradiation by the light irradiation means, the first and second
Voltage applying means for applying a DC voltage with the first working electrode side being a plus side between the electrode films of the working electrode, and generating hydrogen at the electrode film of the second working electrode. I do.
【０００７】この電圧印加に際しては、２Ｖ未満の直流
電圧を印加することが望ましい。[0007] When applying this voltage, it is desirable to apply a DC voltage of less than 2V.
【０００８】上記構成を有する本発明の第１の水素生成
方法とその装置では、第１作用極の電極膜への光照射に
より、当該電極膜の光触媒に触媒活性を起こし、正孔と
電子を生成する。生成された正孔は、第１作用極の電極
膜に残り、生成した電子は、電圧印加のための配線を通
って第１作用極側から第２作用極側に移動する。In the first method and apparatus for producing hydrogen of the present invention having the above-described structure, the light irradiation on the electrode film of the first working electrode causes the photocatalyst of the electrode film to have a catalytic activity to generate holes and electrons. Generate. The generated holes remain on the electrode film of the first working electrode, and the generated electrons move from the first working electrode side to the second working electrode side through wires for voltage application.
【０００９】こうした正孔・電子生成とその移動によ
り、第２作用極の電極膜では、電子により水分子が還元
されて水素が生成する。その一方、第１作用極の電極膜
では、残った正孔による水分子の酸化もしくはアルコー
ル分子の酸化が起こり、前者では酸素が、後者では二酸
化炭素が生成する。[0009] By the generation and movement of holes and electrons, water molecules are reduced by electrons in the electrode film of the second working electrode to generate hydrogen. On the other hand, in the electrode film of the first working electrode, oxidation of water molecules or oxidation of alcohol molecules occurs due to the remaining holes, and oxygen is generated in the former and carbon dioxide is generated in the latter.
【００１０】このように各作用極での反応を進行させる
上で、生成電子の第２作用極側への移動は、第１作用極
をプラス側とした直流電圧印加により妨げられることは
なく、電圧印加に伴って速やかに且つ継続して起きる。
このため、光触媒により生成された正孔と生成された電
子の再結合を第１作用極の電極膜面（詳しくは、光触媒
表面）で起きにくくでき、正孔と電子を効率的に第１、
第２の作用極に分離させる。よって、第２作用極側での
水素生成の効率を高めることができる。なお、第１作用
極側での酸素生成の効率も高めることができる。As described above, when the reaction at each working electrode proceeds, the movement of the generated electrons to the second working electrode side is not hindered by the application of the DC voltage with the first working electrode being the plus side. It occurs quickly and continuously with the application of voltage.
For this reason, the recombination of the holes generated by the photocatalyst and the generated electrons can be made less likely to occur on the electrode film surface of the first working electrode (specifically, the photocatalyst surface), and the holes and the electrons can be efficiently converted into the first and second electrodes.
Separate to the second working electrode. Therefore, the efficiency of hydrogen generation on the second working electrode side can be increased. The efficiency of oxygen generation on the first working electrode side can also be increased.
【００１１】そして、印加する直流電圧を２ｖ未満とす
ることで、水素生成に対して過大な電力供給を必要が無
くなり、水素生成に伴うエネルギ効率を高めることがで
きる。しかも、この程度の直流電圧は、入手が容易で安
価な乾電池で得ることができるので、装置構成の簡略化
や低コスト化を図ることもできる。By setting the applied DC voltage to less than 2 V, it is not necessary to supply an excessive amount of electric power for hydrogen generation, and the energy efficiency accompanying the hydrogen generation can be increased. Moreover, such a DC voltage can be obtained with an easily available and inexpensive dry battery, so that the device configuration can be simplified and the cost can be reduced.
【００１２】なお、光触媒が二酸化チタン、酸化亜鉛、
酸化バナジウム、酸化タングステン等であれば、これら
を光触媒活性可能な紫外領域の光（紫外線）を照射すれ
ばよく、光照射に当たっては、用いる触媒の特性に合わ
せるだけでよい。二酸化チタンにあっては、特に結晶型
がアナターゼ型のものが光触媒活性、入手の容易さから
好ましい。The photocatalyst is titanium dioxide, zinc oxide,
In the case of vanadium oxide, tungsten oxide, or the like, these may be irradiated with light (ultraviolet light) in an ultraviolet region capable of photocatalytic activation, and the light irradiation may be performed only in accordance with the characteristics of the catalyst used. Among the titanium dioxides, those having a crystal form of anatase are particularly preferred from the viewpoint of photocatalytic activity and availability.
【００１３】この他、本発明は次のような態様とするこ
ともできる。即ち、第１作用極の電極膜を、可視光の照
射を受けると光のエネルギを吸収する色素を担持した前
記光触媒の膜で形成する。この場合、担持する色素は、
前記光触媒が呈する最低空軌道（ＬＵＭＯ）エネルギ準
位よりも低い最低空軌道（ＬＵＭＯ）エネルギ準位を有
するものとされ、第１作用極へは、可視光を照射するよ
うにする。こうした色素としては、ビピリジン金属錯
体、金属ポルフィリン、金属フタロシアニン、或いはこ
れらの誘導体とすることが好ましい。[0013] In addition, the present invention may be in the following modes. That is, the electrode film of the first working electrode is formed of the photocatalyst film supporting a dye that absorbs light energy when irradiated with visible light. In this case, the dye to be supported is
It has a lowest unoccupied orbital (LUMO) energy level lower than the lowest unoccupied orbital (LUMO) energy level exhibited by the photocatalyst, and irradiates the first working electrode with visible light. Such a dye is preferably a bipyridine metal complex, metal porphyrin, metal phthalocyanine, or a derivative thereof.
【００１４】こうした色素を担持した光触媒の電極膜
に、光触媒活性の励起可能な光に替わって可視光が照射
されると、その可視光エネルギが色素に吸収される。こ
れにより、色素（詳しくは、色素構成原子）では、その
電子軌道のうちの最低空軌道（ＬＵＭＯ）の電子が、上
記のエネルギ準位の差により、電極膜の光触媒（詳しく
は、光触媒構成原子）の最低空軌道（ＬＵＭＯ）に移動
する。これにより、電子の移動を受けた光触媒では、色
素からの電子移動に伴い光触媒作用が活性化された状態
が起きる。よって、第１作用極からは、電子が既述した
ように電圧印加のための配線を通って第２作用極側に移
動し、この電子移動に伴い正孔が第１作用極に残る。こ
の結果、第２作用極の電極膜では、電子により水分子が
還元されて水素が生成し、第１作用極の電極膜では、残
った正孔による水分子の酸化もしくはアルコール分子の
酸化が起こり、前者では酸素が、後者では二酸化炭素が
生成する。When the electrode film of a photocatalyst carrying such a dye is irradiated with visible light instead of light capable of exciting photocatalytic activity, the visible light energy is absorbed by the dye. As a result, in the dye (specifically, the constituent atoms of the dye), the electron in the lowest unoccupied orbit (LUMO) of the electron orbits is caused by the difference in the energy level, due to the difference in the energy levels. ) To the lowest free orbit (LUMO). As a result, in the photocatalyst that has received the transfer of electrons, a state in which the photocatalysis is activated with the transfer of electrons from the dye occurs. Therefore, from the first working electrode, electrons move to the second working electrode side through the wiring for voltage application as described above, and holes remain in the first working electrode with the electron movement. As a result, in the electrode film of the second working electrode, water molecules are reduced by electrons to generate hydrogen, and in the electrode film of the first working electrode, oxidation of water molecules or oxidation of alcohol molecules occurs due to remaining holes. The former produces oxygen, and the latter produces carbon dioxide.
【００１５】従って、色素担持を図った光触媒を電極膜
として用いた場合には、太陽光、蛍光灯光等の可視光照
射により、水素生成を起こすことができ、その生成効率
をより高めることもできる。Therefore, when a photocatalyst carrying a dye is used as an electrode film, hydrogen can be generated by irradiation with visible light such as sunlight or fluorescent light, and the generation efficiency can be further increased. .
【００１６】[0016]
【発明の他の態様】本発明は、水を電気分解する方法或
いは装置に適用した態様を採ることも可能である。即
ち、 光の照射を受けると正孔と電子を生成する光触媒
活性を呈する光触媒の膜が電極膜として形成された第１
作用極と、電極触媒作用を果たす電極材料の膜が電極膜
として形成された第２作用極とを、前記水或いは前記電
解質溶液中に浸漬された状態とし、その上で、前記第１
作用極の電極膜に、前記光触媒活性の励起可能な光を照
射すると共に、前記第１と第２の作用極の電極膜間に、
前記第１作用極の側をプラス側にして直流電圧を印加す
る。こうすれば、簡単な構成で効率よく水を電気分解で
きる。Other Embodiments of the Invention The present invention can be applied to a method or an apparatus for electrolyzing water. That is, a photocatalytic film exhibiting photocatalytic activity of generating holes and electrons when irradiated with light is formed as an electrode film.
The working electrode and the second working electrode, in which a film of an electrode material performing an electrode catalyst is formed as an electrode film, are immersed in the water or the electrolyte solution.
While irradiating the electrode film of the working electrode with light capable of exciting the photocatalytic activity, between the electrode films of the first and second working electrodes,
A DC voltage is applied with the first working electrode side being a plus side. In this case, water can be efficiently electrolyzed with a simple configuration.
【００１７】[0017]
【発明の実施の形態】次に、本発明の実施の形態を実施
例に基づき説明する。図１は第１実施例の水素生成装置
１０の模式構成図である。Next, embodiments of the present invention will be described based on examples. FIG. 1 is a schematic configuration diagram of the hydrogen generator 10 of the first embodiment.
【００１８】図示するように、水素生成装置１０は、水
を貯留する反応槽１２に、第１作用極２０と第２作用極
３０とを浸漬させて備え、両作用極を定直流電源４０を
介在して導通する。この場合、定直流電源４０は、第１
作用極２０の側がプラス、第２作用極３０の側がマイナ
スとなるようにして導電ライン４１で繋がれており、ス
イッチ４２の回路閉動作で、両作用極間に一定の直流電
圧を印加する。As shown in the figure, the hydrogen generator 10 is provided with a first working electrode 20 and a second working electrode 30 immersed in a reaction tank 12 for storing water. Conducted by intervening. In this case, the constant DC power supply 40
The working electrode 20 is connected to the conductive line 41 such that the side of the working electrode 20 is positive and the side of the second working electrode 30 is negative, and a constant DC voltage is applied between the two working electrodes by closing the circuit of the switch 42.
【００１９】水素生成装置１０は、可視光を照射するタ
ングステンランプ４４（出力約５００Ｗ）と、当該ラン
プの点灯制御並びにスイッチ４２の開閉制御を行う制御
装置４６とを有する。なお、この制御装置４６は、定直
流電源４０の印加する直流電圧値を調整可能とされてい
る。The hydrogen generator 10 has a tungsten lamp 44 (approximately 500 W output) for irradiating visible light, and a control device 46 for controlling the lighting of the lamp and controlling the opening and closing of the switch 42. The control device 46 can adjust the DC voltage value applied by the constant DC power supply 40.
【００２０】第１作用極２０は、所定形状に切り出した
ガラス基板２１を電極基材として備え、その表面に、酸
化インジウムスズ（ＩＴＯ）を用いて薄膜成形された透
明電極２２を有し、この電極面に、光触媒電極膜２３を
有する。この作用極の制作手順は次の通りである。The first working electrode 20 is provided with a glass substrate 21 cut out into a predetermined shape as an electrode base material, and has on its surface a transparent electrode 22 formed into a thin film using indium tin oxide (ITO). The photocatalyst electrode film 23 is provided on the electrode surface. The procedure for producing this working electrode is as follows.
【００２１】まず、ＩＴＯ製の透明電極２２が薄膜形成
済みのガラス基板２１を準備する。次いで、光触媒とし
ての二酸化チタンの粉末（平均粒径約２μｍ）を水に分
散させたペーストを、スピンコート法等の薄膜形成手法
にて透明電極２２の表面に塗布し（約２０ｃｍ２）、そ
の後、約３００℃以上の焼成温度で焼成する。これによ
り、透明電極２２の電極面上に、二酸化チタン薄膜が光
触媒電極膜２３として形成される。この薄膜形成の際、
ペーストの塗布厚が約１０μｍとなるように調整され
る。First, a glass substrate 21 on which a transparent electrode 22 made of ITO has been formed into a thin film is prepared. Next, a paste obtained by dispersing titanium dioxide powder (average particle size: about 2 μm) as a photocatalyst in water is applied to the surface of the transparent electrode 22 by a thin film forming technique such as spin coating (about 20 cm 2 ), and thereafter And firing at a firing temperature of about 300 ° C. or more. Thus, a titanium dioxide thin film is formed as a photocatalyst electrode film 23 on the electrode surface of the transparent electrode 22. When forming this thin film,
The thickness of the paste is adjusted to be about 10 μm.
【００２２】更に、二酸化チタン薄膜形成済みのガラス
基板２１を、ルテニウム錯体溶液中に浸漬して引き上
げ、乾燥処理に処す。これにより、光触媒電極膜２３を
形成する薄膜における二酸化チタン（光触媒）にルテニ
ウム錯体が担持され、光触媒電極膜２３は、ルテニウム
錯体（色素）を担持した光触媒の膜（電極膜）となる。
これらの工程を経て、第１作用極２０が完成する。この
場合、ルテニウム錯体は、光触媒（二酸化チタン）が呈
する最低空軌道（ＬＵＭＯ）エネルギ準位よりも低い最
低空軌道（ＬＵＭＯ）エネルギ準位を有する。Further, the glass substrate 21 on which the titanium dioxide thin film has been formed is dipped in a ruthenium complex solution, pulled up, and subjected to a drying treatment. As a result, the ruthenium complex is supported on the titanium dioxide (photocatalyst) in the thin film forming the photocatalyst electrode film 23, and the photocatalyst electrode film 23 becomes a photocatalyst film (electrode film) supporting the ruthenium complex (dye).
Through these steps, the first working electrode 20 is completed. In this case, the ruthenium complex has a lowest unoccupied orbital (LUMO) energy level lower than that of the photocatalyst (titanium dioxide).
【００２３】なお、透明電極２２に塗布するペースト
を、二酸化チタン粉末に加えてルテニウム錯体の粉末を
配合・分散させたものとし、透明電極２２へのペースト
塗布・焼成を経て、第１作用極２０を制作するようにす
ることもできる。The paste to be applied to the transparent electrode 22 is prepared by mixing and dispersing a ruthenium complex powder in addition to the titanium dioxide powder, and applying the paste to the transparent electrode 22 and firing the first working electrode 20. Can also be produced.
【００２４】第２作用極３０は、ガラス基板２１とほぼ
同形状に切り出したガラス基板３１とその表面に薄膜形
成された白金電極３２を有する。この白金電極３２は、
真空蒸着法等の薄膜形成手法にて形成される。The second working electrode 30 has a glass substrate 31 cut out in substantially the same shape as the glass substrate 21 and a platinum electrode 32 formed on the surface thereof in a thin film. This platinum electrode 32
It is formed by a thin film forming technique such as a vacuum deposition method.
【００２５】こうして作成した第１作用極２０と第２作
用極３０とを図示しない電極保持基材に固定して機械強
度を確保し、その上で、各作用極の透明電極２２と白金
電極３２とを導電ライン４１で接続する。そして、両作
用極を反応槽１２の水に浸漬させた状態とする。The first working electrode 20 and the second working electrode 30 thus formed are fixed to an electrode holding base (not shown) to secure mechanical strength, and then the transparent electrode 22 and the platinum electrode 32 of each working electrode are secured. Are connected by a conductive line 41. Then, both working electrodes are immersed in the water of the reaction tank 12.
【００２６】上記した構成を有する水素生成装置１０
は、制御装置４６によるタングステンランプ４４の点灯
制御と、スイッチ４２の回路閉制御により、第２作用極
３０で水素を生成し、第１作用極２０で酸素を生成す
る。生成能力については後述する。The hydrogen generator 10 having the above configuration
Generates hydrogen at the second working electrode 30 and oxygen at the first working electrode 20 by the lighting control of the tungsten lamp 44 by the control device 46 and the circuit closing control of the switch 42. The generation capability will be described later.
【００２７】第２実施例の水素生成装置は、上記した第
１実施例の水素生成装置１０と、第１作用極構成とラン
プ構成が相違する。つまり、第２実施例では、透明電極
２２に、色素担持のない二酸化チタンを用いて光触媒電
極膜２３が形成されている。また、ランプは、二酸化チ
タンの光触媒活性を励起可能な約４００ｎｍの紫外線
（出力約５００Ｗ）を発する紫外線ランプ４４とされて
いる。The hydrogen generator of the second embodiment differs from the hydrogen generator 10 of the first embodiment in the first working electrode configuration and the lamp configuration. That is, in the second embodiment, the photocatalyst electrode film 23 is formed on the transparent electrode 22 using titanium dioxide having no dye. The lamp is an ultraviolet lamp 44 that emits ultraviolet light of about 400 nm (output of about 500 W) capable of exciting the photocatalytic activity of titanium dioxide.
【００２８】上記した構成を有する第２実施例の水素生
成装置にあっても、制御装置４６による紫外線ランプ４
４の点灯制御と、スイッチ４２の回路閉制御により、第
２作用極３０で水素を生成し、第１作用極２０で酸素を
生成する。生成能力については後述する。In the hydrogen generator of the second embodiment having the above-described configuration, the control unit 46 controls the ultraviolet lamp 4.
By the lighting control of 4 and the circuit closing control of the switch 42, hydrogen is generated at the second working electrode 30 and oxygen is generated at the first working electrode 20. The generation capability will be described later.
【００２９】ここで、上記の実施例の水素生成装置が有
する水素生成能力について説明する。図２は定直流電源
４０による印加電圧値（直流電圧値）と水素発生量の関
係を示すグラフである。Here, the hydrogen generation capability of the hydrogen generator of the above embodiment will be described. FIG. 2 is a graph showing the relationship between the applied voltage value (DC voltage value) from the constant DC power supply 40 and the amount of generated hydrogen.
【００３０】図２に示すグラフは、第１実施例の水素生
成装置１０について、定直流電源４０の印加電圧値を０
〜２Ｖの範囲で種々調整し、各電圧値の電圧を継続印加
した状況下で、タングステンランプ４４による光照射が
無い場合と有る場合のそれぞれの水素発生量を測定した
結果である。第２実施例についても同様であり、各電圧
値の電圧を継続印加した状況下で、紫外線ランプ４４に
よる光照射が無い場合と有る場合のそれぞれの水素発生
量を測定した結果である。この場合、電圧値ゼロの結果
は、第１、第２の作用電極をただ単に導通しただけの水
素生成の結果（光照射有り・無し）である。なお、ガス
生成量は、図１の各電極から生成したガスをガスクロマ
トグラフィーに導いて、時間当たりの生成量をガスクロ
マトグラフィーで測定した。The graph shown in FIG. 2 shows that the applied voltage value of the constant DC power supply 40 is 0 for the hydrogen generator 10 of the first embodiment.
These are the results of measuring the amount of hydrogen generation in the case where there is no light irradiation by the tungsten lamp 44 and in the case where there is light irradiation under the condition that various adjustments are made in the range of up to 2 V and the voltage of each voltage value is continuously applied. The same applies to the second embodiment, which is a result of measuring the amount of hydrogen generated when there is no light irradiation by the ultraviolet lamp 44 and when there is light irradiation by the ultraviolet lamp 44 under the condition that the voltage of each voltage value is continuously applied. In this case, the result of zero voltage value is the result of hydrogen generation (with / without light irradiation) simply by conducting the first and second working electrodes. In addition, the gas generation amount was measured by introducing the gas generated from each electrode in FIG. 1 to gas chromatography, and measuring the generation amount per time by gas chromatography.
【００３１】この図２から判るように、第１、第２の作
用電極を導通しただけであっても（電圧ゼロ）、光照射
により水素を生成できた。また、光照射が無い場合は、
印加電圧が１Ｖ程度から増加するに連れて、水素生成量
が増える。光照射が無ければ、第１作用極２０は光触媒
活性の無い通常の電極として機能するに過ぎないので、
上記の水素生成の状況は、通常の水の電気分解、つま
り、水中で対向する電極間に電圧を印加させて水を電気
分解する場合に観察される状況と同じである。As can be seen from FIG. 2, even when the first and second working electrodes were merely turned on (zero voltage), hydrogen could be generated by light irradiation. If there is no light irradiation,
As the applied voltage increases from about 1 V, the amount of generated hydrogen increases. Without light irradiation, the first working electrode 20 only functions as a normal electrode without photocatalytic activity,
The situation of the above-mentioned hydrogen generation is the same as the situation observed when normal water is electrolyzed, that is, when water is electrolyzed by applying a voltage between electrodes facing each other in water.
【００３２】ところが、色素担持の光触媒を用いた第１
実施例と、色素担持のない光触媒を用いた第２実施例と
も、２Ｖ未満という僅かな直流電圧を印加するだけで、
電圧ゼロの場合の水素生成量の約１．３〜３倍の水素を
生成でき、水素生成効率を高めることができた。なお、
水の電気分解であるところから、第１作用極２０の側で
の酸素生成効率も同様に高めることができた。However, the first method using a dye-carrying photocatalyst
In both the embodiment and the second embodiment using the photocatalyst having no dye, only a small DC voltage of less than 2 V is applied.
About 1.3 to 3 times the amount of hydrogen generated when the voltage was zero could be generated, and the hydrogen generation efficiency could be increased. In addition,
Owing to the electrolysis of water, the oxygen generation efficiency on the side of the first working electrode 20 could be similarly increased.
【００３３】また、このような効率向上に際して、定直
流電源４０を、その印加電圧値の関係から、乾電池等の
簡便な電源とすることができるので、装置構成を簡略化
できる。しかも、色素担持の光触媒を用いた第１実施例
では、光源をタングステンランプ４４や蛍光灯、或いは
太陽光とすることができるので、この点からも構成の簡
略化を図ることができる。In order to improve the efficiency, the constant DC power supply 40 can be a simple power supply such as a dry battery in view of the applied voltage value, so that the device configuration can be simplified. Moreover, in the first embodiment using the dye-carrying photocatalyst, the light source can be a tungsten lamp 44, a fluorescent lamp, or sunlight, so that the configuration can be simplified from this point as well.
【００３４】なお、電圧が２Ｖとなると光照射の有無に
拘わらずほぼ同じ水素生成量となるのは、この電圧（２
Ｖ）では、第１作用極２０での酸素生成が電圧印加に伴
う水の電気分解自体により起きて、その生成酸素が第１
作用極２０の光触媒電極膜２３への光の到達を妨げ、電
極膜での光触媒活性の影響を無視できるものとなると考
えられる。It is to be noted that when the voltage becomes 2 V, almost the same amount of hydrogen is produced regardless of the presence or absence of light irradiation.
In V), the oxygen generation at the first working electrode 20 is caused by the electrolysis of water accompanying the voltage application, and the generated oxygen is converted to the first working electrode 20.
It is considered that the arrival of light at the working electrode 20 to the photocatalytic electrode film 23 is prevented, and the effect of photocatalytic activity on the electrode film can be ignored.
【００３５】上記のようにして生成した水素および酸素
は、図示しない採集管を得てそれぞれのガス貯留部に集
められ、その後の加圧等を経て、ボンベ内に加圧ガスと
して保管される。こうして得られたガス、例えば水素ガ
スは、水素を燃料ガスとする燃料電池発電装置や、燃料
電池自動車に用いるようにすることができる。The hydrogen and oxygen generated as described above are collected in respective gas reservoirs by obtaining a collecting tube (not shown), and are stored as pressurized gas in a cylinder through subsequent pressurization and the like. The gas thus obtained, for example, hydrogen gas, can be used for a fuel cell power generation device using hydrogen as a fuel gas or a fuel cell vehicle.
【００３６】以上本発明の実施例について説明したが、
本発明は上記の実施例や実施形態になんら限定されるも
のではなく、本発明の要旨を逸脱しない範囲において種
々なる態様で実施し得ることは勿論である。The embodiments of the present invention have been described above.
The present invention is not limited to the above-described examples and embodiments at all, and it goes without saying that the present invention can be implemented in various modes without departing from the gist of the present invention.
【００３７】例えば、上記実施例では、反応槽１２に水
を満たした場合について説明したが、反応槽１２にアル
コールを満たしたり、水やアルコールを溶媒とする電解
質溶液を満たして、これら水溶液から、第１、第２の作
用極間の電圧印加、光照射を経て、水素と酸素、或いは
水素と二酸化炭素を生成するようにもできる。For example, in the above-described embodiment, the case where the reaction tank 12 is filled with water is described. However, the reaction tank 12 is filled with alcohol or an electrolyte solution using water or alcohol as a solvent. Through application of a voltage between the first and second working electrodes and light irradiation, hydrogen and oxygen or hydrogen and carbon dioxide can be generated.
【図１】第１実施例の水素生成装置１０の模式構成図で
ある。FIG. 1 is a schematic configuration diagram of a hydrogen generator 10 according to a first embodiment.
【図２】定直流電源４０による印加電圧値（直流電圧
値）と水素発生量の関係を示すグラフである。FIG. 2 is a graph showing a relationship between an applied voltage value (DC voltage value) by a constant DC power supply 40 and an amount of generated hydrogen.
１０…水素生成装置 １２…反応槽 ２０…第１作用極 ２１…ガラス基板 ２２…透明電極 ２３…光触媒電極膜 ３０…第２作用極 ３１…ガラス基板 ３２…白金電極 ４０…定直流電源 ４１…導電ライン ４２…スイッチ ４４…タングステンランプ ４４…紫外線ランプ ４６…制御装置 DESCRIPTION OF SYMBOLS 10 ... Hydrogen generator 12 ... Reaction tank 20 ... First working electrode 21 ... Glass substrate 22 ... Transparent electrode 23 ... Photocatalytic electrode film 30 ... Second working electrode 31 ... Glass substrate 32 ... Platinum electrode 40 ... Constant DC power supply 41 ... Conduction Line 42 switch 44 tungsten lamp 44 ultraviolet lamp 46 control device
───────────────────────────────────────────────────── フロントページの続き (51)Int.Cl.7 識別記号 ＦＩ テーマコート゛(参考） Ｃ２５Ｂ 9/00 Ｃ２５Ｂ 11/08 Ｚ 11/08 11/10 Ｂ 11/10 9/00 Ａ Ｆターム(参考） 4G069 AA03 BA04A BA04B BA14A BA14B BA48A BB04A BC35A BC54A BC60A CC40 EA07 4K011 AA20 AA25 AA26 AA32 CA04 DA01 DA10 4K021 AA01 BA02 BA06 DA02 DA09 DA13 DC03 ──────────────────────────────────────────────────の Continued on the front page (51) Int.Cl. 7 Identification symbol FI Theme coat ゛ (Reference) C25B 9/00 C25B 11/08 Z 11/08 11/10 B 11/10 9/00 A F term (Reference) 4G069 AA03 BA04A BA04B BA14A BA14B BA48A BB04A BC35A BC54A BC60A CC40 EA07 4K011 AA20 AA25 AA26 AA32 CA04 DA01 DA10 4K021 AA01 BA02 BA06 DA02 DA09 DA13 DC03
Claims (8)
媒とする電解質溶液のいずれかから水素を生成する方法
であって、 光の照射を受けると正孔と電子を生成する光触媒活性を
呈する光触媒の膜が電極膜として形成された第１作用極
と、電極触媒作用を果たす電極材料の膜が電極膜として
形成された第２作用極とを、前記水或いは前記電解質溶
液中に浸漬された状態とする工程Ａと、 前記第１作用極の電極膜に、前記光触媒活性の励起可能
な光を照射すると共に、前記第１と第２の作用極の電極
膜間に、前記第１作用極の側をプラス側にして直流電圧
を印加する工程Ｂとを備え、 前記第２作用極の電極膜で水素を生成することを特徴と
する水素生成方法。1. A method for producing hydrogen from either water or an alcohol or an electrolyte solution using these as a solvent, wherein a film of a photocatalyst exhibiting photocatalytic activity of generating holes and electrons when irradiated with light is provided. A step of immersing the first working electrode formed as an electrode film and the second working electrode formed of an electrode film having an electrode material that performs electrode catalysis in the water or the electrolyte solution; A, and irradiating the electrode film of the first working electrode with light capable of exciting the photocatalytic activity, and adding the first working electrode side between the electrode films of the first and second working electrodes. And a step B of applying a DC voltage to the second working electrode, wherein hydrogen is generated by the electrode film of the second working electrode.
成方法。2. The hydrogen generation method according to claim 1, wherein the step B applies a DC voltage of less than 2V.
方法であって、 前記第１作用極の電極膜は、可視光の照射を受けると光
のエネルギを吸収する色素を担持した前記光触媒の膜で
形成され、前記色素は、前記光触媒が呈する最低空軌道
（ＬＵＭＯ）エネルギ準位よりも低い最低空軌道（ＬＵ
ＭＯ）エネルギ準位を有するものとされ、前記工程Ｂ
は、前記光触媒活性の励起可能な光に替えて、可視光を
前記第１作用極に照射する、水素生成方法。3. The hydrogen generating method according to claim 1, wherein the electrode film of the first working electrode carries a dye that absorbs light energy when irradiated with visible light. And the dye is formed in the lowest unoccupied orbit (LUMO) lower than the lowest unoccupied orbit (LUMO) energy level exhibited by the photocatalyst.
MO) has an energy level, and the step B
Is a method for generating hydrogen, which comprises irradiating the first working electrode with visible light instead of light capable of exciting the photocatalytic activity.
金属フタロシアニン、或いはこれらの誘導体の少なくと
も一つである、水素生成方法。4. The method for producing hydrogen according to claim 3, wherein the dye is a bipyridine metal complex, a metal porphyrin,
A method for producing hydrogen, which is at least one of a metal phthalocyanine and a derivative thereof.
媒とする電解質溶液のいずれかから水素を生成する装置
であって、 光の照射を受けると正孔と電子を生成する光触媒活性を
呈する光触媒の膜が電極膜として形成された第１作用極
と、電極触媒作用を果たす電極材料の膜が電極膜として
形成された第２作用極とを、前記水或いは前記電解質溶
液中に浸漬された状態で備える電極反応槽と、 前記第１作用極の電極膜に、前記光触媒活性の励起可能
な光を照射する光照射手段と、 該光照射手段による光照射の実行の間に、前記第１と第
２の作用極の電極膜間に、前記第１作用極の側をプラス
側にして直流電圧を印加する電圧印加手段とを備え、 前記第２作用極の電極膜で水素を生成することを特徴と
する水素生成装置。5. An apparatus for generating hydrogen from either water or an alcohol or an electrolyte solution using these as a solvent, wherein a film of a photocatalyst having photocatalytic activity of generating holes and electrons when irradiated with light is provided. An electrode comprising a first working electrode formed as an electrode film and a second working electrode formed as an electrode film with a film of an electrode material that performs an electrode catalysis in a state immersed in the water or the electrolyte solution. A reaction vessel, light irradiation means for irradiating the electrode film of the first working electrode with light capable of exciting the photocatalytic activity, and between the execution of light irradiation by the light irradiation means, Voltage applying means for applying a DC voltage with the first working electrode side being a plus side between the electrode films of the working electrode, wherein hydrogen is generated by the electrode film of the second working electrode. Hydrogen generator.
水素生成方法。6. The hydrogen generator according to claim 5, wherein the voltage applying unit applies a DC voltage of less than 2V.
Hydrogen generation method.
装置であって、 前記第１作用極の電極膜は、可視光の照射を受けると光
のエネルギを吸収する色素を担持した前記光触媒の膜で
形成され、前記色素は、前記光触媒が呈する最低空軌道
（ＬＵＭＯ）エネルギ準位よりも低い最低空軌道（ＬＵ
ＭＯ）エネルギ準位を有するものとされ、 前記電圧印加手段は、前記光触媒活性の励起可能な光に
替えて、可視光を前記第１作用極に照射する、水素生成
装置。7. The hydrogen generating apparatus according to claim 4, wherein the electrode film of the first working electrode carries a dye that absorbs light energy when irradiated with visible light. And the dye is formed in the lowest unoccupied orbit (LUMO) lower than the lowest unoccupied orbit (LUMO) energy level exhibited by the photocatalyst.
MO) The hydrogen generating apparatus, wherein the voltage applying means irradiates the first working electrode with visible light instead of light capable of exciting the photocatalytic activity.
金属フタロシアニン、或いはこれらの誘導体の少なくと
も一つである、水素生成装置。8. The hydrogen generator according to claim 7, wherein the dye is a bipyridine metal complex, a metal porphyrin,
A hydrogen generator, which is at least one of a metal phthalocyanine and a derivative thereof.
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| JP2001168418A JP2002356301A (en) | 2001-06-04 | 2001-06-04 | Production method for hydrogen and its apparatus |
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|---|---|---|---|
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2006082801A1 (en) * | 2005-02-02 | 2006-08-10 | Japan Science And Technology Agency | Process for producing gas, process for producing acidic water and alkaline water, and apparatus for producing the same |
| JP2006264992A (en) * | 2005-03-22 | 2006-10-05 | Taiyoko Kenkyusho:Kk | Hydrogen production apparatus utilizing condensation of sunlight |
| KR100699556B1 (en) | 2005-10-12 | 2007-03-26 | 한국에너지기술연구원 | The equipment for producing hydrogen gas by using photocatalyst and biocatalyst |
| JP2007524762A (en) * | 2004-02-18 | 2007-08-30 | ゼネラル・モーターズ・コーポレーション | Method and apparatus for hydrogen generation |
| JP2009219958A (en) * | 2008-03-13 | 2009-10-01 | Central Res Inst Of Electric Power Ind | Oxidative decomposition method using photocatalyst and water purification apparatus |
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2001
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP2007524762A (en) * | 2004-02-18 | 2007-08-30 | ゼネラル・モーターズ・コーポレーション | Method and apparatus for hydrogen generation |
| WO2006082801A1 (en) * | 2005-02-02 | 2006-08-10 | Japan Science And Technology Agency | Process for producing gas, process for producing acidic water and alkaline water, and apparatus for producing the same |
| JPWO2006082801A1 (en) * | 2005-02-02 | 2008-08-07 | 独立行政法人科学技術振興機構 | Gas production method, acidic water and alkaline water production method, and production apparatus thereof |
| JP2006264992A (en) * | 2005-03-22 | 2006-10-05 | Taiyoko Kenkyusho:Kk | Hydrogen production apparatus utilizing condensation of sunlight |
| KR100699556B1 (en) | 2005-10-12 | 2007-03-26 | 한국에너지기술연구원 | The equipment for producing hydrogen gas by using photocatalyst and biocatalyst |
| JP2009219958A (en) * | 2008-03-13 | 2009-10-01 | Central Res Inst Of Electric Power Ind | Oxidative decomposition method using photocatalyst and water purification apparatus |
| JP2010168608A (en) * | 2009-01-21 | 2010-08-05 | Panasonic Corp | Hydrogen production apparatus, hydrogen production method using the same and energy system |
| JP5824363B2 (en) * | 2009-10-21 | 2015-11-25 | ＩＦＴＬ−Ｓｏｌａｒ株式会社 | Photoelectrode material and photovoltaic cell material |
| JP2011200748A (en) * | 2010-03-24 | 2011-10-13 | National Institute Of Advanced Industrial Science & Technology | Catalyst for electrochemical oxidation of alcohol |
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