WO2007021055A1 - Alliage de stockage d'hydrogène et appareil servant à stocker de l'hydrogène utilisant celui-ci - Google Patents

Alliage de stockage d'hydrogène et appareil servant à stocker de l'hydrogène utilisant celui-ci Download PDF

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Publication number
WO2007021055A1
WO2007021055A1 PCT/KR2005/003895 KR2005003895W WO2007021055A1 WO 2007021055 A1 WO2007021055 A1 WO 2007021055A1 KR 2005003895 W KR2005003895 W KR 2005003895W WO 2007021055 A1 WO2007021055 A1 WO 2007021055A1
Authority
WO
WIPO (PCT)
Prior art keywords
hydrogen storage
storage alloy
hydrogen
alloy
mixture
Prior art date
Application number
PCT/KR2005/003895
Other languages
English (en)
Inventor
Tae-Hyung Lee
Chul Jung
Il-Chun Choi
Original Assignee
Daum Energy Co., Ltd.
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
Priority claimed from KR1020050075357A external-priority patent/KR100532231B1/ko
Priority claimed from KR1020050075360A external-priority patent/KR100534078B1/ko
Application filed by Daum Energy Co., Ltd. filed Critical Daum Energy Co., Ltd.
Publication of WO2007021055A1 publication Critical patent/WO2007021055A1/fr

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Classifications

    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F17—STORING OR DISTRIBUTING GASES OR LIQUIDS
    • F17C—VESSELS FOR CONTAINING OR STORING COMPRESSED, LIQUEFIED OR SOLIDIFIED GASES; FIXED-CAPACITY GAS-HOLDERS; FILLING VESSELS WITH, OR DISCHARGING FROM VESSELS, COMPRESSED, LIQUEFIED, OR SOLIDIFIED GASES
    • F17C11/00—Use of gas-solvents or gas-sorbents in vessels
    • F17C11/005—Use of gas-solvents or gas-sorbents in vessels for hydrogen
    • 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
    • C01B3/0005—Reversible uptake of hydrogen by an appropriate medium, i.e. based on physical or chemical sorption phenomena or on reversible chemical reactions, e.g. for hydrogen storage purposes ; Reversible gettering of hydrogen; Reversible uptake of hydrogen by electrodes
    • 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
    • Y02E60/32—Hydrogen storage

Definitions

  • the present invention relates, in general, to a hydrogen storage alloy comprising an
  • the present invention relates to an apparatus for storing hydrogen at room temperature under low pressure, comprising a cylindrical body having an internal charging space of a predetermined capacity, a valve unit disposed to transfer a fluid between the inside and outside of the body, a filtering unit connected to the valve unit and having a porous conduit, a plurality of heat conducting members, each of which has one end connected to the filtering unit to be radially disposed around the filtering unit, and a hydrogen storage alloy included in the body while contacting the heat conducting member.
  • the above alloy suffers because the alloy components are homogenized for use thereof and also are pulverized at high temperatures to increase the surface area thereof.
  • Hydrogen storage methods include four types, that is, adsorption of hydrogen to gas, liquid and activated carbon, and storage of hydrogen to a hydrogen storage alloy.
  • such a reactor 50 includes a reaction container 51 having a predetermined volume, a flow conduit 52, having a hydrogen flow passage 52a, provided in the container, a plurality of flow prevention plates 56 parallely disposed to be spaced apart from each other by a predetermined interval around the flow conduit 52 and each having a plurality of holes 54 in a manner such that holes of an upper flow prevention plate 56 have a diameter smaller than those of a lower flow prevention plate 56, a hydrogen storage alloy 53 charged in the reaction container 51, and a filter 55 provided to the upper portion of the flow conduit 52.
  • the hydrogen storage alloy reactor includes the hydrogen storage alloy with a small diameter at the upper portion thereof and the hydrogen storage alloy with a large diameter at the lower portion thereof, in order to store external hydrogen in the storage container 51. Further, the charging density of the hydrogen storage alloy is uniformly distributed depending on the diameter by the flow prevention plates 56, thus controlling heat generated by the upper and lower portions thereof.
  • An object of the present invention is to provide a hydrogen storage alloy, which easily realizes activation, increases the storage amount of hydrogen, decreases hysteresis upon hydrogen storage, functions at room temperature under low pressure, has good heat conductivity, and increases the storage and discharge amounts of hydrogen.
  • Another object of the present invention is to provide an apparatus for storing hydrogen using a hydrogen storage alloy, which has a simple structure, increases the strength of the tank itself, is easily used, has low manufacturing cost and excellent heat exchange performance, is operable at room temperature under low pressure, and rapidly charges the alloy thanks to easy heat exchange.
  • the present invention provides a hydrogen storage alloy, which is represented by ReNi V M , in which Re is a rare earth metal, M is a misch metal, 1.35 ⁇ x ⁇ 1.65, 0.1 ⁇ y ⁇ 0.4, and 0.05 ⁇ z ⁇ 0.25.
  • the present invention provides an apparatus for storing hydrogen using a hydrogen storage alloy, comprising a cylindrical body having an internal charging space of a predetermined capacity sealed by an upper cover and a lower cover; a valve unit connected to the upper cover to transfer a fluid between the inside and outside of the body; a filtering unit connected to the valve unit and having a porous conduit; and a plurality of heat conducting members, each of which has one end connected to the filtering unit to be radially disposed around the filtering unit so as to have the maximum contact area with the hydrogen storage alloy.
  • a hydrogen storage alloy can easily realize activation, increase the storage amount of hydrogen, decrease hysteresis upon hydrogen storage, function at room temperature under low pressure, have good heat conductivity, and increase the storage and discharge amounts of hydrogen.
  • an apparatus for storing hydrogen using the hydrogen storage alloy can have a simple structure, increase the strength of the tank itself, be easily used, have low manufacturing cost and excellent heat exchange performance, be operated at room temperature under low pressure, and rapidly charge the alloy thanks to easy heat exchange.
  • FIG. 1 is a cross-sectional view showing a conventional hydrogen storage alloy reactor using a hydrogen storage alloy
  • FIG. 2 is a cross-sectional view showing a hydrogen storage container according to a first embodiment of the present invention
  • FIGS. 3 and 4 are cross-sectional views showing a hydrogen storage container according to a second embodiment of the present invention
  • FIG. 5 is a perspective view showing a hydrogen storage container according to a third embodiment of the present invention
  • FIGS. 6 and 7 are perspective views showing a hydrogen storage container according to a fourth embodiment of the present invention
  • FIG. 8 is a graph showing the storage amount of the hydrogen storage alloy prepared in Example 2 of the present invention
  • FIG. 9 is a graph showing the storage amount of the hydrogen storage alloy prepared in Example 3 of the present invention
  • FIG. 10 is a graph showing the properties of the alloy varying with the atomic ratios of the alloy of the present invention.
  • Re is a rare earth metal
  • M is a misch metal
  • Re which is a rare earth metal, comprises a mixture of La, Ce, Pr, and Nd.
  • M which is a mesch metal, comprises a mixture of Co, Mn, Al and Fe.
  • the misch metal such as Co, Mn, Al and Fe, is added to the above metal elements, thereby increasing the hydrogen storage efficiency at room temperature.
  • the hydrogen storage alloy comprises 6.0-10.0 wt% of La, 15.0-19.0 wt% of Ce,
  • 3.0-5.0 wt% of Zr may be replaced with 3.0-5.0 wt% of Co.
  • M is a hydrogen storage alloy prepared by melting the metal mixture.
  • the alloy is subjected to activation treatment, in which the activation treatment is conducted by repeating processes of applying high-pressure hydrogen into a vacuum chamber and then discharging it several times.
  • La, Ce, Pr and Nd which are known for their properties, are basically used, along with Ni, to constitute an AB type of alloy as a fundamental hydrogen storage alloy.
  • the hydrogen storage amount varies with the amounts of V, Zr (Co), Mn, Al and
  • the value of x is which is the most reasonably applicable is selected, and the values of y and z are controlled through application of the calculated data. Thereby, while the physical properties of the alloy are not changed, the hydrogen storage amount of the alloy can be increased. The value of x is uniformly applied based on the experimental results.
  • V and Fe are important elements between hydrogen and metal. Although Fe has low reactivity with hydrogen, Fe can function to control the reactivity between hydrogen and the other elements to improve the activation performance of the alloy. [59] Further, when the alloy absorbs hydrogen, the absorption of hydrogen is promoted and the absorption pressure of hydrogen is decreased. Upon discharge of hydrogen, the discharge speed is increased, thus forming a predetermined pressure. [60] Co functions to prevent pulverization of the hydrogen alloy. Instead of Co, Zr may be used. [61] As such, Zr functions to enhance the bondability between hydrogen and the other elements and greatly increase the hydrogen storage amount of the hydrogen storage alloy so as to improve the activation conditions.
  • Mn functions to control the pressure equilibrium upon the reaction between the alloy and hydrogen. If excess Mn is used, it negatively affects the fusibility of the other elements, resulting in decreased alloy properties. Thus, the amount of Mn is preferably limited to 2 wt% or less.
  • Al functions to increase the reactivity of hydrogen and the lifetime of hydrogen storage alloy, and to decrease the hydrogen absorption pressure at room temperature.
  • Al since Al may malfunction to inhibit the diffusion of hydrogen and decrease the storage amount of alloy, its amount is limited to 1.2 wt% or less.
  • the hydrogen storage amount of the alloy thus prepared was 0.9 wt%.
  • the amount of each element was 8.0 wt% of La, 17.0 wt% of Ce, 1.5 wt% of Pr, 4.5 wt% of Nd, 48.0 wt% of Ni, 12.0 wt% of V, 4.0 wt% of Co, 3.0 wt% of Mn, 1.0 wt% of Al and 0.3 wt% of Fe.
  • the alloy had 1.8 wt% of hydrogen storage amount, as shown in a graph of hydrogen storage amount depending on the pressure and temperature of hydrogen of FIG. 8.
  • the amount of each element was 8.0 wt% of La, 17.0 wt% of Ce, 1.5 wt% of Pr, 4.5 wt% of Nd, 48.0 wt% of Ni, 13.0 wt% of V, 4.0 wt% of Zr, 1.0 wt% of Mn, 1.0 wt% of Al and 1.3 wt% of Fe.
  • the alloy had 3.4 wt% of hydrogen storage amount, as shown in a graph of hydrogen storage amount depending on the pressure and temperature of hydrogen of FIG. 9, in which V and Fe were used to control the reactivity between hydrogen and metal and V was regarded as an important element among the hydrogen storage alloy.
  • Fe having low reactivity with hydrogen, was used to control the reaction between hydrogen and the other element in order to improve activation performance of the alloy, promote the hydrogen absorption of the alloy, and decrease the absorption pressure of hydrogen.
  • Zr was used to enhance the bondability between hydrogen and the other metal, increase the storage amount of the hydrogen storage alloy, and improve the activation.
  • the alloy of the present example resulting from replacing Co with Zr and increasing the amounts of V and Fe among the alloy components of Example 1, could store 3.4 wt% of hydrogen at room temperature (2O 0 C) under low pressure (1.5 MPa).
  • the apparatus of the present invention comprises a body
  • the body 100 is cylindrical shape and has an internal charging space of a predetermined capacity, and the internal charging space in the body is sealed by an upper cover and a lower cover joined to upper and lower ends of the body through welding.
  • the valve unit 200 is connected to the upper cover to transfer a predetermined pressure of hydrogen between the inside and outside of the body 100, and further includes a pressurization part 230 connected at one side thereof and a plug member 250 disposed to be pressed to an inlet of the body 100 so as to introduce and discharge hydrogen therethrough.
  • the filtering unit 300 is connected to the valve unit 200 and includes a porous conduit 310 for flow of hydrogen gas therethrough.
  • the plurality of heat conducting members 400 is radially disposed around the porous conduit 310.
  • the heat conducting members 400 are longitudinally extended along a length of the body 100 and radially connected to the conduit 310 to be spaced apart from each other by a predetermined angular interval.
  • the heat conducting members 400 may be arranged along a length of the body to be spaced from each other by a predetermined linear interval in a plurality of groups and connected to the conduit 310 to be spaced apart from each other by a predetermined angular interval.
  • the heat conducting members 400 may have a plurality of protrusions provided thereon while maintaining the configuration of being longitudinally extended along a length of the body 100 and radially connected to the conduit 310 to be spaced apart from each other by a predetermined angular interval.
  • the heat conducting members 400 may have a plurality of protrusions provided thereon and may be curved with respect to a radial direction while maintaining the configuration of being longitudinally extended along a length of the body 100 and radially connected to the conduit 310 to be spaced apart from each other by a predetermined angular interval.
  • the hydrogen storage alloy 500 is charged in the body to closely contact the lateral sides of the heat conducting member 400.
  • the hydrogen storage alloy 500 may be integrally attached to the heat conducting member 400.
  • the hydrogen storage alloy comprises, based on the total weight of the hydrogen storage alloy, 6.0-10.0 wt% of La, 15.0-19.0 wt% of Ce, 1.2-1.8 wt% of Pr, 4.1-4.9 wt% of Nd, 43.4-52.6 wt% of Ni, 11.0-15.0 wt% of V, 3.0-5.0 wt% of Zr, 0.5-2.0 wt% of Mn, 0.5-1.2 wt% of Al, and 1.5-1.7 wt% of Fe, and thus can store 2-4 wt% of hydrogen.
  • the filtering unit 300 which has the plurality of heat conducting members 400 radially connected to the outer surface thereof, is inserted into the body 100 formed of aluminum as removing the upper cover, after which the upper cover is joined to the body using welding.
  • the upper cover, joined to the upper end of the body 100, is opened without the valve unit 200 connected thereto, and the hydrogen storage alloy 500 having a predetermined size is charged into the body through the opened portion.
  • the heat conducting member 400 may be formed by being integrally compressed to the body 100. At this time, the filtering unit 300 may be inserted into the central portion of the body to assemble it.
  • valve unit 200 When the hydrogen storage alloy 500 is completely charged, the valve unit 200 is connected to the upper cover. As such, the valve unit 200 is threadly coupled to the upper cover while applying an adhesive therebetween such that the body 100 is maintained in a state of being sealed while the valve unit may be opened and closed to enable hydrogen to flow therethrough.
  • valve unit 200 When the valve unit 200 is opened, external hydrogen is supplied, thereby adsorbing such hydrogen to the hydrogen storage alloy.
  • the filtering unit 300 is formed of stainless steel and has a hydrogen gas flow groove having a diameter of 20 D or less such that hydrogen can be stored and discharged under predetermined pressure.
  • the heat conducting member 400 is formed to have a plurality of protrusions provided thereon or a curved shape so as to maximize the contact area with the alloy without interference with the alloy to be charged in a longitudinal direction of the body 100, thus having the maximum area per unit diameter.
  • the valve unit 200 further includes a separate pressurization part 230 to supply hydrogen gas under various pressures, if required.
  • the present invention provides a hydrogen storage alloy which enables a hydrogen storage apparatus to be operated at room temperature under lower pressure, has good heat conductivity, and increases hydrogen absorption and discharge amounts.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • Inorganic Chemistry (AREA)
  • Filling Or Discharging Of Gas Storage Vessels (AREA)
  • Fuel Cell (AREA)

Abstract

Alliage de stockage d'hydrogène et appareil servant à stocker de l'hydrogène utilisant celui-ci. Précisément, l'alliage de stockage d'hydrogène est un alliage d'hydrogène à base de (RE)Nix-y-zVyMz où RE est un métal des terres rares, M est un mischmétal, 1,35≤x≤1,65, 0,1≤y≤0,4 et 0,05≤z≤0,25. En plus, l'appareil servant à stocker de l'hydrogène à température ambiante et à basse pression comprend un corps ayant un couvercle supérieur et un couvercle inférieur et un espace de chargement ayant une capacité déterminée définie par le couvercle supérieur et le couvercle inférieur ; une partie soupape reliée au couvercle supérieur pour transférer un fluide entre l'intérieur et l'extérieur du corps ; une partie filtration reliée à la partie soupape et ayant une tuyauterie poreuse ; et une pluralité d'éléments conducteurs de chaleur, chacun desquels ayant une extrémité reliée à la partie filtration pour maximiser la surface de contact avec l'alliage de stockage d'hydrogène à charger.
PCT/KR2005/003895 2005-08-17 2005-11-17 Alliage de stockage d'hydrogène et appareil servant à stocker de l'hydrogène utilisant celui-ci WO2007021055A1 (fr)

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
KR1020050075357A KR100532231B1 (ko) 2005-08-17 2005-08-17 수소가스 저장장치
KR10-2005-0075357 2005-08-17
KR10-2005-0075360 2005-08-17
KR1020050075360A KR100534078B1 (ko) 2005-08-17 2005-08-17 수소저장합금

Publications (1)

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WO2007021055A1 true WO2007021055A1 (fr) 2007-02-22

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Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2014500787A (ja) * 2010-10-20 2014-01-16 コールドウェイ 複合材料製ジャケットを有する熱化学系
US9234264B2 (en) 2004-12-07 2016-01-12 Hydrexia Pty Limited Magnesium alloys for hydrogen storage
CN105387341A (zh) * 2015-11-18 2016-03-09 北京有色金属研究总院 一种金属氢化物储氢罐
US9435489B2 (en) 2010-02-24 2016-09-06 Hydrexia Pty Ltd Hydrogen release system
CN107270120A (zh) * 2017-07-05 2017-10-20 长安大学 一种车载轻质高压金属氢化物复合式储氢罐
CN107859871A (zh) * 2016-09-22 2018-03-30 全球能源互联网研究院 一种金属氢化物储氢装置及其储存金属氢化物的方法
US11141784B2 (en) 2015-07-23 2021-10-12 Hydrexia Pty Ltd. Mg-based alloy for hydrogen storage

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS60135541A (ja) * 1983-12-23 1985-07-18 Agency Of Ind Science & Technol 水素貯蔵合金
JPS61207529A (ja) * 1985-03-12 1986-09-13 Aisin Seiki Co Ltd 水素貯蔵合金の製造方法
JPH0873970A (ja) * 1994-09-09 1996-03-19 Sumitomo Metal Ind Ltd 水素吸蔵合金とこれを用いたＮｉ−水素電池用負極
JPH09194971A (ja) * 1996-01-10 1997-07-29 Japan Steel Works Ltd:The 水素吸蔵材料
US6197448B1 (en) * 1997-05-30 2001-03-06 Duracell Inc. Hydrogen storage alloy

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS60135541A (ja) * 1983-12-23 1985-07-18 Agency Of Ind Science & Technol 水素貯蔵合金
JPS61207529A (ja) * 1985-03-12 1986-09-13 Aisin Seiki Co Ltd 水素貯蔵合金の製造方法
JPH0873970A (ja) * 1994-09-09 1996-03-19 Sumitomo Metal Ind Ltd 水素吸蔵合金とこれを用いたＮｉ−水素電池用負極
JPH09194971A (ja) * 1996-01-10 1997-07-29 Japan Steel Works Ltd:The 水素吸蔵材料
US6197448B1 (en) * 1997-05-30 2001-03-06 Duracell Inc. Hydrogen storage alloy

Cited By (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9234264B2 (en) 2004-12-07 2016-01-12 Hydrexia Pty Limited Magnesium alloys for hydrogen storage
US9435489B2 (en) 2010-02-24 2016-09-06 Hydrexia Pty Ltd Hydrogen release system
US10215338B2 (en) 2010-02-24 2019-02-26 Hydrexia Pty Ltd. Hydrogen release system
JP2014500787A (ja) * 2010-10-20 2014-01-16 コールドウェイ 複合材料製ジャケットを有する熱化学系
US9486763B2 (en) 2010-10-20 2016-11-08 Societe Coldway Thermochemical system having a housing made of a composite material
US11141784B2 (en) 2015-07-23 2021-10-12 Hydrexia Pty Ltd. Mg-based alloy for hydrogen storage
CN105387341A (zh) * 2015-11-18 2016-03-09 北京有色金属研究总院 一种金属氢化物储氢罐
CN107859871A (zh) * 2016-09-22 2018-03-30 全球能源互联网研究院 一种金属氢化物储氢装置及其储存金属氢化物的方法
CN107270120A (zh) * 2017-07-05 2017-10-20 长安大学 一种车载轻质高压金属氢化物复合式储氢罐
CN107270120B (zh) * 2017-07-05 2020-04-10 长安大学 一种车载轻质高压金属氢化物复合式储氢罐

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