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WO2008001489A1 - Générateur d'hydrogène et procédé de génération d'hydrogène - Google Patents

Générateur d'hydrogène et procédé de génération d'hydrogène Download PDF

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Publication number
WO2008001489A1
WO2008001489A1 PCT/JP2007/000669 JP2007000669W WO2008001489A1 WO 2008001489 A1 WO2008001489 A1 WO 2008001489A1 JP 2007000669 W JP2007000669 W JP 2007000669W WO 2008001489 A1 WO2008001489 A1 WO 2008001489A1
Authority
WO
WIPO (PCT)
Prior art keywords
hydrogen
aqueous solution
acidic aqueous
deuterium
discharge
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.)
Ceased
Application number
PCT/JP2007/000669
Other languages
English (en)
Japanese (ja)
Inventor
Yoshiro Tanaka
Tadahiko Mizuno
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
OCT Inc
Original Assignee
OCT Inc
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by OCT Inc filed Critical OCT Inc
Priority to JP2008522296A priority Critical patent/JPWO2008001489A1/ja
Publication of WO2008001489A1 publication Critical patent/WO2008001489A1/fr
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/06—Combination of fuel cells with means for production of reactants or for treatment of residues
    • H01M8/0606—Combination of fuel cells with means for production of reactants or for treatment of residues with means for production of gaseous reactants
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B3/00—Hydrogen; Gaseous mixtures containing hydrogen; Separation of hydrogen from mixtures containing it; Purification of hydrogen
    • C01B3/02—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen
    • C01B3/04—Production of hydrogen or of gaseous mixtures containing a substantial proportion of hydrogen by decomposition of inorganic compounds, e.g. ammonia
    • 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

Definitions

  • the present invention relates to a method and apparatus for generating a gas containing hydrogen.
  • Patent Document 1 a hydrogen generation apparatus including a hydrogen generation tank configured to store an acidic aqueous solution and to be able to immerse a metal having a higher ionization tendency than hydrogen in the acidic aqueous solution. Proposed.
  • Patent Document 2 hydrogen gas production in which hydrogen gas is generated by bringing a single metal into contact with a deuterium acidic aqueous solution in which at least some of the hydrogen atoms in the acidic aqueous solution are substituted with deuterium atoms. A method has been proposed.
  • Non-Patent Document 1 discloses a technique for generating a gas containing hydrogen by causing plasma electrolysis in an atmosphere containing droplets containing deuterium. is suggesting.
  • Patent Document 1 Japanese Unexamined Patent Publication No. 2003-20202
  • Patent Document 2 International Publication No. 02Z066368
  • Non-Patent Document 1 Tadahiko Mizuno et al., “Hydrogen Evolution by Plasma Electrolysis in Aqueous Solution”, Journal of Japan Society of Applied Physics, 44 (1 A), 2005
  • Non-Patent Document 1 the plasma generator used in the technique proposed in Non-Patent Document 1 has a complicated structure and is expensive, and there is still room for improvement from the viewpoint of obtaining a hydrogen-containing gas at a low cost. Hot.
  • an object of the present invention is to provide a hydrogen generation method capable of generating a large amount of hydrogen-containing gas at a lower cost.
  • Another object of the present invention is to provide a hydrogen generation apparatus that can be suitably used for such a hydrogen generation method.
  • the present invention provides:
  • a holding unit for holding an acidic aqueous solution containing deuterium
  • a hydrogen generator is provided.
  • an acidic aqueous solution containing deuterium can be more easily and efficiently decomposed with low energy by using inexpensive deuterium and water as raw materials and an apparatus having a simple configuration. Can produce a large amount of hydrogen (hydrogen-containing gas) at low cost.
  • the present invention also provides a hydrogen generation method that can be suitably performed using the hydrogen generation apparatus. That is, the present invention
  • a method for producing hydrogen is also provided.
  • an acidic aqueous solution containing deuterium can be more easily and efficiently decomposed with low energy by using inexpensive deuterium and water as raw materials and a device having a simple configuration.
  • the hydrogen generator further includes a heating device, a spraying device, or an ultrasonic generator, and the atomized acidic solution in the space portion by the heating device, the spraying device, or the ultrasonic generator. It is preferable to form an atmosphere containing an aqueous solution. In particular, in the step (1), it is preferable to form a mist atmosphere containing the acidic aqueous solution.
  • the acidic aqueous solution can be more reliably present in a place where discharge occurs (for example, a discharge path), and hydrogen can be generated more efficiently.
  • the discharge device is preferably an arc discharge generator that causes arc discharge. That is, in the above step (2)
  • the voltage required to start the arc discharge is relatively high, but since the sustain voltage is low, hydrogen can be generated at a lower cost.
  • the acidic aqueous solution used in the hydrogen generator and the hydrogen generation method preferably contains D 2 0, and preferably contains D 2 S 0 4 .
  • the present inventors have found that hydrogen can be generated more efficiently when the acidic aqueous solution contains a deuterium component. The reason is not clear However, we believe that excess energy is generated by the transmutation reaction near the tip of the electrode where arc discharge occurs, and a large amount of hydrogen can be generated.
  • the pH of the acidic aqueous solution is preferably 2.0 to 3.5.
  • FIG. 1 is a schematic cross-sectional view showing an embodiment of a hydrogen generator of the present invention.
  • FIG. 2 is a schematic cross-sectional view of the hydrogen generator of the present invention used in the examples.
  • FIG. 1 is a schematic sectional view showing a preferred embodiment of the hydrogen generator of the present invention. First, the configuration of the hydrogen generator 1 of the present invention shown in FIG. 1 will be described.
  • a hydrogen generator 1 shown in FIG. 1 includes a holding unit 4 that holds an acidic aqueous solution 2 containing deuterium, a space 6 that forms an atmosphere containing an acidic aqueous solution, and an upper part 8 of the space 6.
  • a discharge device (including a positive electrode 8a and a negative electrode 8b) for causing a discharge to generate a hydrogen-containing gas.
  • the hydrogen generator 1 of the present embodiment includes an atmosphere forming device 10 including a cellular container for forming an atmosphere including the acidic aqueous solution 2.
  • the cellular container can be opened at least partially with respect to the holding part 4 and contains an acidic aqueous solution.
  • acidic aqueous solution 2 containing deuterium various acidic aqueous solutions containing deuterium as one component can be used.
  • Acid components contained in the acidic aqueous solution 2 include, for example, inorganic acids such as sulfuric acid, hydrochloric acid and nitric acid, as well as citrate, glycine, gay cinnamate, succinate, salicylic acid, formic acid, glutamic acid, and And organic acids such as rubic acid, oxalic acid, tartaric acid, lactic acid and acetic acid. Two or more of these acid components may be contained in the acidic aqueous solution 2, or an inorganic acid and an organic acid may be contained in combination.
  • deuterium in which some hydrogen atoms are replaced with deuterium atoms
  • bisulfuric acid in which some hydrogen atoms are substituted with deuterium atoms
  • an acid component such as dutrium tellurium (D 2 S) is contained in the acidic aqueous solution 2 as a deuterium component.
  • an acidic aqueous solution 2 preferably contains at least one heavy hydrogen component of D 2 0 and D 2 S0 4 0. 5 ⁇ 1 0 vol%.
  • the present inventors have found through experiments that more hydrogen can be generated when a discharge occurs in a mist atmosphere of the acidic aqueous solution 2. That is, if it is 0.5 volume% or more, hydrogen can be generated more reliably, and if it is 10 volume% or less, it is preferable from the viewpoint of cost reduction.
  • the acidic aqueous solution 2 preferably contains 0.5 to 5.0% by volume of at least one deuterium component of D 2 0 and D 2 S0 4 . Within this range, hydrogen can be generated more reliably and at low cost.
  • the deuterium component is D 2 S0 4 .
  • the acidic aqueous solution contains a deuterium component, so that excess energy is generated by the transmutation reaction near the tip of the electrode where arc discharge occurs, and a large amount of hydrogen can be generated.
  • S in D 2 S0 4 acts as a catalyst on the surface of the anode 8 a, the surface of the anode 8 a acts as a reactant, a transmutation reaction occurs, and a large amount of hydrogen gas is generated. It is considered a thing.
  • conductive materials such as various metals can be used.
  • platinum is preferably used from the viewpoint of high reactivity.
  • the acidic aqueous solution 2 may be acidic (about pH 7 or less), but the pH is preferably about 2.0 to about 3.5, for example. In such a range, Hydrogen can be generated more reliably when a discharge occurs in a foggy atmosphere of the acidic aqueous solution 2.
  • thermoplastic resin such as a fluororesin such as polytetrafluoroethylene (PTFE), an inorganic material such as glass, or a metal material such as aluminum, titanium, or an alloy thereof.
  • PTFE polytetrafluoroethylene
  • metal material such as aluminum, titanium, or an alloy thereof.
  • the holding part 2 in FIG. 1 has a bottomed cylindrical shape, has a concave vertical section, and has an opening above, but is sealed with the above-described fluororesin cap 2a.
  • the material constituting the cap 2 a preferably has chemical resistance that does not deteriorate due to the acidic aqueous solution 2.
  • An atmosphere forming device 10 made of a cellular container is connected to the space 6 so that an atmosphere containing the acidic aqueous solution 2 is formed in the space 6 (step (1)). Therefore, the atmosphere forming device 10 includes not only the above-described cellular container but also a heating device, a spraying device, an ultrasonic generator, etc., although not shown. What is important is to form an atmosphere containing an acidic aqueous solution in the holding part 4 (particularly an atmosphere containing a mist-like acidic aqueous solution).
  • an atmosphere containing the acidic aqueous solution in the holding portion 4 it is important to form an atmosphere containing the acidic aqueous solution in the holding portion 4 (particularly, an atmosphere containing a mist-like acidic aqueous solution) and cause discharge in the atmosphere.
  • a discharge may be generated in the atmosphere.
  • the amount of electric power is small and the reaction efficiency can be increased as compared with the conventional discharge in an aqueous solution.
  • the cellular container may be omitted, and a heating device, a spray device, or an ultrasonic generator may be provided inside or outside the holding unit 4.
  • a heating device, a spray device, or an ultrasonic generator may be provided inside or outside the holding unit 4.
  • an atmosphere forming device 10 composed of a cellular container is provided in the holding unit 4, but the cellular container is omitted, and the holding unit 4 itself is installed on a magnetic stirrer with a heating device.
  • a fogging device may be connected to the holding unit 4 or an ultrasonic transducer may be connected to the holding unit 4 for connection.
  • the acidic aqueous solution 2 can be gasified (vaporized) by heating, and an atmosphere containing the gasified acidic aqueous solution 2 can be formed in the space 6. Further, according to the spraying device, the acidic aqueous solution 2 can be supplied (sprayed) in the space 6 in the form of a mist. Furthermore, according to the ultrasonic generator, the acidic aqueous solution 2 can be gasified (vaporized) by applying ultrasonic vibration to form an atmosphere containing the gasified acidic aqueous solution 2 in the space 6.
  • a discharge device including an anode 8 a and a cathode 8 b is provided in the upper portion 8 of the space 6.
  • deuterium contained in the acidic aqueous solution 2 is decomposed to generate hydrogen by causing discharge (step (2)).
  • the discharge device it is preferable to use a discharge device capable of generating arc discharge.
  • Any arc discharge generator may be used as long as it can generate arc discharge between the anode 8a and the cathode 8b, and a conventionally known apparatus can be used.
  • Examples of the discharge include arc discharge, glow discharge, and plasma discharge.
  • the discharge is low in voltage and safe, and a versatile discharge device can be used to efficiently generate hydrogen. From the viewpoint of being able to do so, the present inventors decided to adopt arc discharge.
  • the voltage and current density between the electrodes at the time of discharge may be appropriately selected within a range that does not impair the effect of the present invention. it may be set, the current density is, for example, 1 0 0-1 may be set to OOO AZ cm 2.
  • the temperature of the atmosphere can be increased by the heat of reaction without any particular heating. Therefore, a cooling device may be provided, and the ambient temperature remains at room temperature. However, from the viewpoint of improving the reactivity, it is preferable that the temperature of the atmosphere is higher.
  • the temperature is controlled to be 70 ° C to 100 ° C, and 70 ° C to 80 ° C. preferable.
  • the reaction can proceed even if the pressure in the atmosphere is not particularly increased, it is preferably controlled to a high pressure from the viewpoint of increasing the reaction efficiency. For example, it can be controlled to 3 0 0 to 5 0 0 at m. Also, the supercritical state may be formed by controlling the temperature and pressure.
  • the gas containing hydrogen generated by the above discharge moves along the direction of arrow Y through the pipe 9 connected to the upper portion 8.
  • a gas flow meter a mass spectrum analyzer, a hydrogen collector, etc. at the tip of the pipe 9.
  • a condensing unit is provided so as to cover the pipe 9, and the water contained in the gas containing hydrogen is condensed and removed by flowing a cooling fluid such as cooling water. May be. In this way, a highly pure hydrogen-containing gas can be obtained.
  • a hydrogen generator having the structure shown in FIG. 2 was produced to generate hydrogen.
  • a holding unit 4 made of a bottomed cylindrical container made of polytetrafluoroethylene and having an opening with a diameter of 7 cm was prepared, and the container was placed on a magnetic stirrer equipped with a heating device.
  • the heating device served as the atmosphere forming device 10.
  • the opening of the holding portion 4 was closed with a rubber cap 2a made of Teflon (registered trademark).
  • the cap 2a is provided with a through-hole, and in order to capture the gas generated in the holding part 4, a quartz glass pipe 9 is passed through the through-hole, and the space part 6 of the pipe 9 is relatively in the middle.
  • a large part (upper part) 8 was formed, and a Tandastain anode 8a and a tungsten cathode 8b were installed.
  • the upper end of the pipe 9 Connect a Tygon tube with a diameter of 8 mm (not shown) to the end of the arrow Y, and connect the gas flow meter (model 31 00 made by Coflock Co., Ltd.) and the control unit (model CR made by Coffrock Co., Ltd.) —700) is connected, and a mass spectrum analyzer (Rega_20 made by ULVAC, Inc.) is installed downstream of the gas flowmeter.
  • the acidic aqueous solution 2 containing 0.25 vol% of 0 2 50 4 is placed, and the temperature of the heating device located at the bottom of the holding unit 4 is set to 85 ° C to generate steam of the acidic aqueous solution 2 I let you. Then, a voltage of 30000 V is intermittently applied between the anode 8 a and the cathode 8 b, a current of 0.37 to 4.3 mA is passed, and arc discharge is performed in the vapor of the acidic aqueous solution 2. Formed.
  • the hydrogen generation device and the hydrogen generation method of the present invention a large amount of hydrogen can be obtained in a short time at a low cost.
  • a fuel cell, a hydrogen gas driving device, and a hydrogen self-charging turbocharger In addition, it can be suitably used for hydrogen gas supply in a cogeneration system using an electric vehicle using a hydrogen self-sufficient turbocharger.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Sustainable Energy (AREA)
  • Sustainable Development (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Fuel Cell (AREA)

Abstract

L'invention concerne un générateur d'hydrogène qui permet de beaucoup de gaz contenant de l'hydrogène à un coût inférieur. L'invention concerne également un procédé pour générer de l'hydrogène. L'invention concerne de façon spécifique un générateur d'hydrogène comprenant une section de contenant pour contenir une solution aqueuse acide contenant un composant de deutérium, une section d'espace pour former une atmosphère contenant la solution aqueuse acide, et un dispositif de décharge électrique pour générer un gaz contenant de l'hydrogène en provoquant une décharge électrique dans la section d'espace. En particulier, D2SO4 est utilisé comme composant de deutérium, et une décharge à arc est utilisée comme décharge électrique.
PCT/JP2007/000669 2006-06-27 2007-06-21 Générateur d'hydrogène et procédé de génération d'hydrogène Ceased WO2008001489A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP2008522296A JPWO2008001489A1 (ja) 2006-06-27 2007-06-21 水素生成装置および水素生成方法

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2006-176612 2006-06-27
JP2006176612 2006-06-27

Publications (1)

Publication Number Publication Date
WO2008001489A1 true WO2008001489A1 (fr) 2008-01-03

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JP (1) JPWO2008001489A1 (fr)
WO (1) WO2008001489A1 (fr)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2010147495A1 (fr) * 2009-06-18 2010-12-23 Viorel Bucur Installation de traitement des eaux
WO2012011499A1 (fr) * 2010-07-20 2012-01-26 Ishikawa Yasuo Procédé de transformation nucléaire et dispositif de transformation nucléaire
JP2014025743A (ja) * 2012-07-25 2014-02-06 Ti:Kk 核変換方法
JP2019183240A (ja) * 2018-04-13 2019-10-24 住友金属鉱山株式会社 カドミウム回収設備および回収方法

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH08109002A (ja) * 1994-02-28 1996-04-30 Hokushin Ind Inc 水素ガス製造装置
WO2002066368A1 (fr) * 2001-02-22 2002-08-29 Yoshirou Tanaka Procede de production d'hydrogene
JP2003340437A (ja) * 2002-05-23 2003-12-02 Toshiyasu Sato 水の燃焼方法
JP2004059977A (ja) * 2002-07-26 2004-02-26 Tadahiko Mizuno 水素ガスの発生方法および水素ガス発生装置

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH08109002A (ja) * 1994-02-28 1996-04-30 Hokushin Ind Inc 水素ガス製造装置
WO2002066368A1 (fr) * 2001-02-22 2002-08-29 Yoshirou Tanaka Procede de production d'hydrogene
JP2003340437A (ja) * 2002-05-23 2003-12-02 Toshiyasu Sato 水の燃焼方法
JP2004059977A (ja) * 2002-07-26 2004-02-26 Tadahiko Mizuno 水素ガスの発生方法および水素ガス発生装置

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
MIZUNO T. ET AL.: "Hydrogen Evolution by Plasma Electrolysis in Aqueous Solution", JAPANESE JOURNAL OF APPLIED PHYSICS, vol. 44, no. 1A, 2005, pages 396 - 401, XP003020326 *

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2010147495A1 (fr) * 2009-06-18 2010-12-23 Viorel Bucur Installation de traitement des eaux
WO2012011499A1 (fr) * 2010-07-20 2012-01-26 Ishikawa Yasuo Procédé de transformation nucléaire et dispositif de transformation nucléaire
JP2014025743A (ja) * 2012-07-25 2014-02-06 Ti:Kk 核変換方法
JP2019183240A (ja) * 2018-04-13 2019-10-24 住友金属鉱山株式会社 カドミウム回収設備および回収方法
JP6992662B2 (ja) 2018-04-13 2022-01-13 住友金属鉱山株式会社 カドミウム回収設備および回収方法

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