WO2013021508A1 - 水素精製装置及びその使用方法 - Google Patents

水素精製装置及びその使用方法 Download PDF

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Publication number
WO2013021508A1
WO2013021508A1 PCT/JP2011/068634 JP2011068634W WO2013021508A1 WO 2013021508 A1 WO2013021508 A1 WO 2013021508A1 JP 2011068634 W JP2011068634 W JP 2011068634W WO 2013021508 A1 WO2013021508 A1 WO 2013021508A1
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WO
WIPO (PCT)
Prior art keywords
hydrogen
gas
mixed fluid
oxygen
flow path
Prior art date
Application number
PCT/JP2011/068634
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English (en)
French (fr)
Japanese (ja)
Inventor
中西　治通
中村　徳彦
英一 有川
弘文 藤原
久保　秀人
藤　敬司
明子 熊野
祥平 松本
Original Assignee
トヨタ自動車株式会社
株式会社豊田自動織機
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 トヨタ自動車株式会社, 株式会社豊田自動織機 filed Critical トヨタ自動車株式会社
Priority to CN201180072811.7A priority Critical patent/CN103748034B/zh
Priority to PCT/JP2011/068634 priority patent/WO2013021508A1/ja
Priority to DE112011105521.8T priority patent/DE112011105521B4/de
Priority to JP2013527834A priority patent/JP5648748B2/ja
Publication of WO2013021508A1 publication Critical patent/WO2013021508A1/ja

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    • 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
    • C01B3/50—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification
    • C01B3/501—Separation of hydrogen or hydrogen containing gases from gaseous mixtures, e.g. purification by diffusion
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/22—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols by diffusion
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B13/00—Oxygen; Ozone; Oxides or hydroxides in general
    • C01B13/02—Preparation of oxygen
    • C01B13/0229—Purification or separation processes
    • C01B13/0248—Physical processing only
    • C01B13/0251—Physical processing only by making use of membranes
    • 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
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2256/00—Main component in the product gas stream after treatment
    • B01D2256/12—Oxygen
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2256/00—Main component in the product gas stream after treatment
    • B01D2256/16—Hydrogen
    • 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

Definitions

  • the present invention relates to a hydrogen purifier obtained by purifying hydrogen from a mixed fluid containing gaseous hydrogen, gaseous oxygen and liquid water, and in particular purifies hydrogen from a mixed fluid containing bubbles of gaseous hydrogen and gaseous oxygen in liquid water.
  • the present invention relates to a hydrogen purification apparatus to be obtained.
  • the present invention also relates to a method for purifying and producing hydrogen using this hydrogen purifier.
  • Japanese Patent Application Laid-Open No. 2004-35356 and Japanese Patent Application Laid-Open No. 2004-292284 propose using a hydrogen separation membrane that selectively allows only hydrogen to permeate.
  • Japanese Patent Application Laid-Open No. 2008-207969 proposes the use of a hydrogen separation membrane for separating hydrogen from a mixed gas obtained by steam reforming using a hydrocarbon fuel.
  • the present invention provides a hydrogen purifier that efficiently purifies hydrogen from a mixed fluid containing gaseous hydrogen, gaseous oxygen, and liquid water.
  • the present invention also provides a method for purifying and producing hydrogen using this hydrogen purifier.
  • the hydrogen purifier of the present invention is a mixed fluid flow path through which a mixed fluid containing gaseous hydrogen, gaseous oxygen and liquid water flows; a mixed fluid which is adjacent to the mixed fluid flow path and contains gaseous hydrogen and gaseous oxygen First gas flow path through which gas flows; Second gas flow path adjacent to the first gas flow path and through which gaseous hydrogen or oxygen flows; Mixed fluid flow path and first gas flow A gas-liquid separation membrane that constitutes at least a part of a wall surface between the channel and separates the mixed gas from the mixed fluid of the mixed fluid channel and provides the mixed gas to the first gas channel; and the first Forming at least a part of a wall surface between the gas flow path and the second gas flow path, and separating gaseous hydrogen or oxygen from the mixed gas of the first gas flow path to form the second gas A hydrogen or oxygen separation membrane is provided for the flow path.
  • FIG. 1 is a diagram for explaining a first aspect of the hydrogen purification apparatus of the present invention.
  • FIG. 2 is a diagram for explaining a second aspect of the hydrogen purification apparatus of the present invention.
  • FIG. 3 is a diagram showing an example of a mixed fluid flow path of the hydrogen purification apparatus of the present invention.
  • FIG. 4 is a diagram showing another example of the mixed fluid flow path of the hydrogen purification apparatus of the present invention.
  • the hydrogen purifier of the present invention is used for purifying and obtaining hydrogen from a mixed fluid containing gaseous hydrogen, gaseous oxygen and liquid water. More specifically, in the hydrogen purifier of the present invention, a gas mixture containing gaseous hydrogen and gaseous oxygen is separated from a fluid mixture containing gaseous hydrogen, gaseous oxygen and liquid water by a gas-liquid separation membrane, and this Hydrogen or oxygen is separated from the mixed gas by a hydrogen or oxygen separation membrane to obtain hydrogen.
  • a mixed fluid containing gaseous hydrogen, gaseous oxygen and liquid water can be obtained, for example, by decomposing water, in particular by electrolyzing water. And gaseous oxygen bubbles.
  • this hydrogen purification apparatus of the present invention before hydrogen or oxygen is separated from a mixed gas containing gaseous hydrogen and gaseous oxygen by the hydrogen or oxygen separating membrane, gaseous hydrogen, gaseous oxygen and Liquid water can be separated from the mixed fluid containing liquid water. According to this, it is possible to suppress the formation of a water film on the hydrogen or oxygen separation membrane, thereby suppressing the decrease in hydrogen or oxygen separation efficiency due to the water film on the hydrogen or oxygen separation membrane.
  • the gas-liquid separation membrane constitutes at least a part of the wall surface above the mixed fluid flow path in order to promote the separation of the mixed gas by the gas-liquid separation membrane.
  • the pressure of the mixed fluid channel is larger than the pressure of the first gas channel, and the pressure of the first gas channel is the second It can be made larger than the pressure of the gas flow path.
  • the specific pressure depends on the operating temperature of the hydrogen purification apparatus of the present invention, the separation performance and strength of the membrane to be used, etc., for example, the pressure of the mixed fluid channel is set to 1 atm or more, and the first gas channel The pressure is less than 1 atm and 0.01 atm or more, and the partial pressure in the second gas channel of hydrogen or oxygen separated by the hydrogen or oxygen separation membrane is the same as that in the first gas channel of hydrogen or oxygen. It is particularly preferable that the pressure be smaller than the partial pressure.
  • a part of hydrogen and / or oxygen can be taken out from the mixed fluid in advance by another apparatus.
  • the remaining hydrogen and / or part of oxygen can be taken out from the mixed fluid by another apparatus.
  • Examples of other hydrogen purifiers in this case include container-type gas-liquid separators that use gravity, centrifugal force, and the like.
  • the mixed fluid after being processed by the hydrogen purifying apparatus of the present invention and optional other apparatus is substantially composed of water, and therefore is discarded and / or decomposed again to form gaseous hydrogen, gaseous oxygen. And a mixed fluid containing liquid water.
  • the “gas-liquid separation membrane” used in the present invention is an arbitrary membrane that can selectively permeate gaseous hydrogen and gaseous oxygen as gaseous components from a mixed fluid containing gaseous hydrogen, gaseous oxygen and liquid water. Can be used.
  • the molar ratio ⁇ (H 2 + O 2 ) / H 2 O ⁇ between the permeation amount of gaseous hydrogen and gaseous oxygen and the permeation amount of liquid water is, for example, 2 or more, 10 or more, 50 or more, 100 or more at the operating temperature. Or 1,000 or more.
  • gas-liquid separation membranes are known.
  • a porous ceramic body having a water-repellent coating can be used.
  • an air-permeable support such as a porous ceramic body or a metal mesh laminated on a gas-liquid separation membrane.
  • the “hydrogen separation membrane” used in the present invention any membrane capable of preferentially permeating hydrogen over oxygen from a mixed gas containing gaseous hydrogen and gaseous oxygen can be used.
  • the molar ratio (H 2 / O 2 ) between the hydrogen permeation amount and the oxygen permeation amount may be, for example, 2 or more, 10 or more, 50 or more, 100 or more, or 1,000 or more at the operating temperature. .
  • oxygen separation membrane used in the present invention, any membrane capable of preferentially permeating oxygen over hydrogen from a mixed gas containing gaseous hydrogen and gaseous oxygen can be used.
  • the molar ratio (O 2 / H 2 ) between the oxygen permeation amount and the hydrogen permeation amount may be, for example, 2 or more, 10 or more, 50 or more, 100 or more, or 1,000 or more at the operating temperature. .
  • oxygen separation membranes are known.
  • Japanese Patent Application Laid-Open No. 2008-062188 can be referred to.
  • an oxygen separation membrane made of a composite oxide having a mixed conductor of oxygen ions and electrons such as CaTiO 3 can be used.
  • the hydrogen purifier of the present invention in the first aspect, is a mixed fluid flow path in which a mixed fluid containing gaseous hydrogen, gaseous oxygen and liquid water flows; adjacent to the mixed fluid flow path; A first gas channel through which a mixed gas containing gaseous oxygen flows; a second gas channel adjacent to the first gas channel and through which gaseous hydrogen flows; a mixed fluid channel and a first gas channel A gas-liquid separation membrane that forms at least a part of a wall surface between the first gas flow path and separates the mixed gas from the mixed fluid in the mixed fluid flow path and provides the separated gas to the first gas flow path And at least part of the wall surface between the first gas flow path and the second gas flow path, and separating the gaseous hydrogen from the mixed gas of the first gas flow path, A hydrogen separation membrane is provided to the gas flow path.
  • the mixed fluid (H 2 + O 2 + H 2 O) is supplied to the mixed fluid channel (12), and the gaseous component (H 2 + O 2 ) of the mixed fluid is supplied to the wall surface between the mixed fluid channel and the first gas channel.
  • a gas-liquid separation membrane (13) constituting at least a part of the gas and provided to the first gas flow path (14) to provide a mixed gas (H 2 + O 2) containing gaseous hydrogen and gaseous oxygen.
  • hydrogen in the mixed gas (H 2 + O 2 ) is formed into a hydrogen separation membrane (at least part of the wall surface between the first gas flow path and the second gas flow path ( 15) and provided to the second gas flow path (16).
  • hydrogen can be obtained from the second gas channel (16). Note that the fraction obtained from the first gas flow path (14) is discarded as a fraction containing a relatively large amount of oxygen, recirculated to further extract hydrogen, and used for other purposes. Can do so.
  • the first aspect is that it is easy to reduce the amount of oxygen mixed into the obtained hydrogen by recovering as hydrogen the gas component that has permeated the hydrogen separation membrane that separates oxygen and hydrogen. preferable.
  • an oxygen separation membrane is used instead of the hydrogen separation membrane of the first aspect.
  • the oxygen separation membrane constitutes at least a part of the wall surface of the first gas flow path, and separates the gaseous oxygen from the mixed gas of the first gas flow path, so that the second gas flow path To provide.
  • a gas-liquid separation membrane (23) constituting at least a part of the wall surface and provided to the first gas flow path (24) to provide a mixed gas (H 2 + O containing gaseous hydrogen and gaseous oxygen) 2 ), and oxygen in the mixed gas (H 2 + O 2 ) constitutes at least a part of a wall surface between the first gas channel and the second gas channel.
  • a gas-liquid separation membrane (23) constituting at least a part of the wall surface and provided to the first gas flow path (24) to provide a mixed gas (H 2 + O containing gaseous hydrogen and gaseous oxygen) 2 ), and oxygen in the mixed gas (H 2 + O 2 ) constitutes at least a part of a wall surface between the first gas channel and the second gas channel.
  • hydrogen can be obtained from the first gas flow path (24).
  • the fraction obtained from the second gas flow path (26) is discarded as a fraction containing a relatively large amount of oxygen, recirculated to further extract hydrogen, and used for other purposes. Can do so.
  • this second aspect is preferable in that the amount of gas that must pass through a gas separation membrane that separates oxygen and hydrogen can be relatively reduced.
  • the mixed fluid flow path of the hydrogen purification apparatus of the present invention can have a separation promoting mechanism for promoting separation of gaseous hydrogen and gaseous oxygen from liquid water.
  • a separation promoting mechanism for promoting separation of gaseous hydrogen and gaseous oxygen from liquid water.
  • An example of such a separation promoting mechanism is a mechanism as shown in FIGS.
  • the gas-liquid separation membrane (13) constitutes at least a part of the wall surface vertically above the mixed fluid channel (12), and the mixed fluid channel ( 12) has a mixed gas collecting member (51) extending downward from the vertically upper wall surface of the mixed fluid flow path, whereby the mixed gas collecting member (51) flows through the mixed fluid flow path.
  • a mixed gas containing hydrogen and oxygen, particularly bubbles (42) of the mixed gas is collected from the mixed fluid and brought into contact with the gas-liquid separation membrane (13).
  • the gas mixture, particularly the bubbles of the mixed gas, contained in the mixed fluid flowing through the mixed fluid flow path is held by the gas collecting member, and the gas-liquid separation membrane and the gas Contact with hydrogen and gaseous oxygen can be ensured, thereby facilitating separation of gaseous hydrogen and gaseous oxygen from the mixed fluid by the gas-liquid separation membrane.
  • the mixed gas collecting member is obliquely lowered toward the flow direction of the mixed fluid in the mixed fluid flow path as shown in FIG. 3 in order to promote the collection of the mixed gas contained in the mixed fluid. It may extend to. In addition, the mixed gas collecting member may particularly extend substantially perpendicular to the direction of the flow of the mixed fluid in the mixed fluid flow path or obliquely downward along the direction of the flow.
  • the mixed fluid flow path has a stirring mechanism (61) for stirring the mixed fluid.
  • the mixed gas bubbles (42) contained in the mixed fluid flowing in the mixed fluid channel (12) and the gas-liquid separation can be promoted, thereby promoting the separation of the mixed gas from the mixed fluid by the gas-liquid separation membrane.
  • the hydrogen purifier as shown in FIG. 4 it is possible to promote a relatively large bubble by combining a plurality of bubbles contained in the mixed fluid.
  • This stirring mechanism is particularly suitable for promoting the contact between the gas bubbles (42) of the mixed gas contained in the mixed fluid and the gas-liquid separation membrane (13) as shown by the arrow (62) in FIG.
  • the mixed fluid in the flow path may be able to flow toward the gas-liquid separation membrane (13).
  • the mixed fluid supplied to the hydrogen purification apparatus of the present invention may be a mixed fluid obtained by any method.
  • the mixed fluid may be a mixed fluid obtained by decomposition of water, in particular direct thermal decomposition, thermochemical decomposition, or photocatalytic decomposition of water. The decomposition of these waters will be described below.
  • Direct thermal decomposition of water is the most basic method for decomposing water to obtain hydrogen and oxygen, and is a method for directly decomposing water into hydrogen and oxygen at a high temperature of several thousand degrees Celsius. This reaction originally requires a temperature of several thousand degrees Celsius, but can be achieved at a temperature around 2,000 degrees Celsius by using a catalyst.
  • thermochemical decomposition method of water is a method in which water is decomposed at a lower temperature than in the case of direct thermal decomposition by combining chemical reactions.
  • Thermochemical decomposition methods especially thermochemical decomposition methods using redox reactions between metals and metal oxides, or thermochemical decomposition methods using redox reactions between metal oxides with different oxidation states can be scaled up. Yes, the prospects for practical use are on the rise.
  • thermochemical decomposition method using a redox reaction between a metal and a metal oxide includes a redox reaction between a metal such as magnesium (Mg), aluminum (Al), iron (Fe) and the metal oxide.
  • a method of using is known.
  • thermochemical decomposition method using a redox reaction between metal oxides having different oxidation states a method using a redox reaction of iron oxides having different oxidation states is known.
  • an IS (iodine-sulfur) cycle method is known as another thermochemical decomposition method.
  • the water photocatalytic decomposition method is a method of decomposing water into hydrogen and oxygen by irradiating light to a photocatalyst such as titanium oxide in contact with water.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Analytical Chemistry (AREA)
  • Combustion & Propulsion (AREA)
  • Health & Medical Sciences (AREA)
  • General Health & Medical Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Oil, Petroleum & Natural Gas (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Separation Using Semi-Permeable Membranes (AREA)
  • Hydrogen, Water And Hydrids (AREA)
PCT/JP2011/068634 2011-08-11 2011-08-11 水素精製装置及びその使用方法 WO2013021508A1 (ja)

Priority Applications (4)

Application Number Priority Date Filing Date Title
CN201180072811.7A CN103748034B (zh) 2011-08-11 2011-08-11 氢精制装置及其使用方法
PCT/JP2011/068634 WO2013021508A1 (ja) 2011-08-11 2011-08-11 水素精製装置及びその使用方法
DE112011105521.8T DE112011105521B4 (de) 2011-08-11 2011-08-11 Vorrichtung zum Aufbereiten von Wasserstoff und Verfahren zum Verwenden derselben
JP2013527834A JP5648748B2 (ja) 2011-08-11 2011-08-11 水素精製装置及びその使用方法

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Application Number Priority Date Filing Date Title
PCT/JP2011/068634 WO2013021508A1 (ja) 2011-08-11 2011-08-11 水素精製装置及びその使用方法

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WO2013021508A1 true WO2013021508A1 (ja) 2013-02-14

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CN (1) CN103748034B (zh)
DE (1) DE112011105521B4 (zh)
WO (1) WO2013021508A1 (zh)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP7385616B2 (ja) 2021-03-22 2023-11-22 株式会社日本トリム 電解水生成装置

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Publication number Priority date Publication date Assignee Title
CN105692549A (zh) * 2014-11-28 2016-06-22 中国科学院大连化学物理研究所 制备高纯度氢气的系统及方法
CN106186210A (zh) * 2016-08-30 2016-12-07 周锋 一种饮用水装置
DE102018221447A1 (de) * 2018-12-11 2020-06-18 Friedrich-Alexander-Universität Erlangen-Nürnberg Verfahren und Anlage zum Freisetzen von Gas aus einem flüssigen Medium
CN110127606A (zh) * 2019-06-26 2019-08-16 张朝林 一种水高温分解为氢气和氧气的方法及分离器

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP7385616B2 (ja) 2021-03-22 2023-11-22 株式会社日本トリム 電解水生成装置

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JPWO2013021508A1 (ja) 2015-03-05
CN103748034B (zh) 2015-10-21
CN103748034A (zh) 2014-04-23
DE112011105521B4 (de) 2018-12-13
DE112011105521T5 (de) 2014-05-08
JP5648748B2 (ja) 2015-01-07

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