EP2051931A2 - Procédé et dispositif pour stocker et libérer de l'hydrogène - Google Patents

Procédé et dispositif pour stocker et libérer de l'hydrogène

Info

Publication number
EP2051931A2
EP2051931A2 EP07784619A EP07784619A EP2051931A2 EP 2051931 A2 EP2051931 A2 EP 2051931A2 EP 07784619 A EP07784619 A EP 07784619A EP 07784619 A EP07784619 A EP 07784619A EP 2051931 A2 EP2051931 A2 EP 2051931A2
Authority
EP
European Patent Office
Prior art keywords
hydrogen
water
reaction
micro
hollow spheres
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.)
Withdrawn
Application number
EP07784619A
Other languages
German (de)
English (en)
Inventor
Marcus Keding
Martin Tajmar
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.)
FOTEC Forschungs- und Technologietransfer GmbH
Original Assignee
Austrian Research Centers GmbH ARC
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 Austrian Research Centers GmbH ARC filed Critical Austrian Research Centers GmbH ARC
Publication of EP2051931A2 publication Critical patent/EP2051931A2/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • 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; Reversible storage of hydrogen
    • C01B3/0005—Reversible storage of hydrogen, e.g. by hydrogen getters or electrodes
    • C01B3/001—Reversible storage of hydrogen, e.g. by hydrogen getters or electrodes characterised by the uptaking media; Treatment thereof
    • 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; Reversible storage of hydrogen
    • C01B3/02—Production of hydrogen; Production of gaseous mixtures containing hydrogen
    • C01B3/06—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen with inorganic reducing agents
    • C01B3/065—Production of hydrogen; Production of gaseous mixtures containing hydrogen by reaction of inorganic compounds containing electro-positively bound hydrogen with inorganic reducing agents by reaction of inorganic compounds with hydrides
    • 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
    • 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
    • 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 new method for storing and targeted release of hydrogen and a new system for carrying out the method.
  • the present invention relates to the hydrogen storage of a new type of gas withdrawal procedure from hydrogen filled microspheres.
  • An essential novel feature of the invention is the coating of the hydrogen-filled microspheres with a small amount of a specific catalyst to control the reaction between water that fills the interstices between the microspheres and a hydrogen in bonded form and the same upon contact to accelerate water-releasing substance, in particular sodium borohydride or sodium borohydride on the micro-spherical surface, which is provided by this reaction necessary for the permeability of the walls of the micro-spheres heat energy in the smallest space.
  • a specific catalyst to control the reaction between water that fills the interstices between the microspheres and a hydrogen in bonded form and the same upon contact to accelerate water-releasing substance, in particular sodium borohydride or sodium borohydride on the micro-spherical surface, which is provided by this reaction necessary for the permeability of the walls of the micro-spheres heat energy in the smallest space.
  • the invention thus relates to a method for storing and deliberately releasing hydrogen according to the European Patent Application Publication No. Hei f f of the copending European Patent Application Publication No. He, which comprises the method cited in the preamble of this claim.
  • Another essential object of the invention is a new device for storage and release of hydrogen for a wide range of applications, which is based in particular on the new hydrogen storage and - release method.
  • the generation and use of hydrogen for a variety of purposes and tasks is increasingly discussed and used to a small extent, with the advantage that hydrogen in a huge extent in the form of free and bound Water is available on the ground, and that when it is burned or reacted with oxygen, which runs very clean, again water is formed, so that practically the source of water can not be lost.
  • the worldwide attempts of the use of hydrogen as an inexhaustible source of energy, and in particular in view of the expected in any case bottlenecks in supplying the world with fossil fuels, in particular with oil and natural gas.
  • great problems still pose the most secure handling of hydrogen and in particular the compact storage of this energy source for the various fields of application, and in particular for mobile objects, such as motor vehicles.
  • Hydrogen has the disadvantage over natural gas, which is in increasing use, that it can liquefy only at very low temperatures and can thus be stored in gaseous form only in highly stable pressure vessels.
  • the hydrogen storage density of hydrogen-filled micro-glass beads is very high, but there is one major drawback: heating the beads takes a lot of energy and time.
  • the use of the waste heat of e.g. a powered with the hydrogen from the micro-spheres fuel cell requires a complex heat exchanger circuit between the fuel cell and the storage tank.
  • the packing density of the micro-spheres of only 60% is a great disadvantage.
  • NaBH 4 sodium borohydride
  • Storage of hydrogen herein is based on the catalytic hydrolysis of the sodium borohydride, which is a per se easy-to-handle liquid, and the byproduct of the hydrolysis reaction, sodium boron oxide, can ultimately be recycled to sodium borohydride with the aid of hydrogen.
  • the temperature at the end of this hydrolysis reaction should reach about 270 0 C in order to optimize or maximize the hydrogen release from the MIKROE balls. It has been found that by using catalysts, the temperature of the microspheres can be lowered to ambient temperature while still releasing 7% by weight of hydrogen from the microspheres.
  • An essential aspect of the invention relates to the coating of the microspheres, each with a small amount of effective catalyst to accelerate the reaction between the hydrogen-containing substance, ie between the hydride and water on the surface of the microspheres. It is achieved a very accelerated hydrolysis reaction and thus finally an accelerated and concentrated in the smallest space and sufficient heat production. In the new way, the micro-sphere walls are locally heated directly by the hydrolysis reaction and become permeable to the hydrogen trapped in the microspheres.
  • Another important aspect of the invention relates to the hydrolysis reaction as a heat supplier.
  • the microsphere / water mixture is brought into contact with sodium borohydride in the reaction chamber and the heat generated during the reaction serves for the release of the hydrogen from the microspheres.
  • the waste products of the reaction consisting essentially of sodium boroxide and empty microspheres, are collected in a separate container.
  • the entire hydrogen storage capacity of the new plant is through the
  • the activation energy for conventional hydrogen-filled glass beads is usually 55kJ / mol, whereby the micro-ball bed is heated to about 27O 0 C. This results in a required amount of sodium borohydride of 0.2 moles and a required amount 0.4 mol of water to heat 1 mol of the microspheres to 270 ° C.
  • the minimum volume of water is 0.4 cm 3 per cm 3 scoops in order to bring the "packing density" to 100% and to increase.
  • NaBH 4 to 1 cm 3 H 2 O to 1 cm 3 microspheres each based on the volume, or 1.04 g NaBH 4 to 1 g H 2 O to 0.36 g microspheres, each based on the Dimensions.
  • the theoretical storage capacity of the system is 11, 75 wt .-% hydrogen at a storage pressure of 700 bar within the balls.
  • the realistic ratios are 0.90 to 1, 10 g of NaBH 4 to 0.95 to 10.5 g of H 2 O to 0.30 to 0.40 g of hydrogen with micro-spheres containing 700 bar.
  • the sodium boron oxide formed in the heat-generating reaction can be recycled to sodium borohydride in a simple chemical process, and the empty microspheres can be refilled with hydrogen.
  • the present invention provides a convenient solution for transportation, storage and provision of hydrogen.
  • the corresponding solutions currently used, such as compressed and liquid hydrogen, are not without danger, they require a large volume at high weight and are not long-term stable.
  • the proposed invention leads to a substantial reduction in volume, weight and energy consumption and to a significant improvement in safety.
  • US 6746496 A describes the prevention of the formation of a crust in the reaction of sodium borohydride with water in the presence of a catalyst by using micro or nano-particles of both the sodium borohydride and the catalyst.
  • catalyst coated glass microspheres are used to cause hydrogen formation on the surface of the spheres to provide the heat needed to release the hydrogen from the glass microspheres. Prevention of the formation of a crust through the glass microspheres is not intended. Furthermore, it is not intended that the sodium borohydride particles are coated with a catalyst, nor should the catalyst be present as a nanoparticle free.
  • This US-A further describes the use of the released in the reaction of hydrogen and oxygen in a fuel cell water for the reaction with sodium borohydride.
  • the use of water as the reaction product e.g. a fuel cell not received.
  • Water and glass microspheres form only one component of the system, the other component is sodium borohydride.
  • WO 1998/021772 A1 describes the release of gas from glass microspheres by breaking the same.
  • the gas is released by diffusion through the glass wall of the glass microspheres. This process is assisted or accelerated by supplying heat.
  • the procedure according to the invention thus enables a non-destructive removal of gas from glass microspheres. After emptying these glass beads, they can be filled with gas again, so they are recyclable.
  • US 2004052723 A1 describes the production of hydrogen by the hydrolysis of water and solid sodium borohydride, which are stored separately from each other. Here it is necessary to heat the water to at least 120 c C to start the reaction.
  • a solution of sodium borohydride, sodium hydroxide and water was used.
  • This solution can release hydrogen only in the presence of a suitable catalyst. Heating of the solution is not required. The heat released by the exothermic reaction is used to release the hydrogen from the glass microspheres.
  • alkaline, alkaline-earth and complex metal hydrides can also generate hydrogen by adding water, thereby releasing heat.
  • these include, in particular, substances such as alanates, boranates and the simple hydrides, Alanates of the type Ax (AlH 4 ) y , where A is an alkali metal or alkaline earth metal, primarily sodium, lithium, magnesium...
  • Al aluminum and H is hydrogen, boronates of Type A x (BH 4 ) y, where A is an alkali or alkaline earth metal, B is boron and H is hydrogen and / or simple hydrides of the type A x H y1 where A is an alkali metal and H is hydrogen and x and y are integers, where x is preferably 1 and y is preferably 1 or 2.
  • Typical hydrides are, for example, NaH, LiH, MgH 2 .
  • solutions of sodium borohydride typically
  • a base typically 0.01-20%, primarily NaOH, and water, also referred to as “stable solutions”.
  • stable solutions are stable for a long time and can produce hydrogen in the presence of suitable catalysts.
  • the abovementioned metal hydrides can also form a stable solution with water and a suitable base, especially NaOH, and produce hydrogen and heat in the presence of a suitable catalyst.
  • any hydride is suitable which can release hydrogen and heat with water and a suitable catalyst, with liquids or stable solutions being particularly well suited due to their very good handleability.
  • Pure metals, such as Silicon or aluminum can also be used for this reaction because under certain circumstances, such as increased pressure, temperature, presence of NaOH in silicon, and presence of gallium in aluminum, they can split the hydrogen out of the water while releasing heat.
  • the invention relates to the reprocessing of the end products obtained in the context of the reaction provided for in accordance with the invention, such as oxides and "empty" microspheres.
  • claim 10 has a new plant or device for storing and releasing hydrogen, which in particular according to operates the new hydrogen storage and release process and has the features appearing in the local flag.
  • the invention relates to the novel catalyst-coated hydrogen-filled microspheres.
  • the present invention supports an innovative gas sampling procedure for
  • Micro-glass balls without supply of external energy.
  • the gas sampling procedure is based on the temperature dependence of the diffusion. As the temperature of the sphere is increased, so does the permeability of the glass wall to hydrogen. The heat required is provided by the hydrolysis reaction of sodium borohydride.
  • coating the microspheres with a small amount of the specific catalyst results in the substantially accelerated hydrolysis reaction on the surface of the hollow sphere wall and thus in the desired accelerated gas production.
  • Fig. 1 shows schematically a section through one of the filled with hydrogen under high pressure micro-hollow spheres
  • Fig. 2 is a diagram of the method according to the invention and at the same time the new hydrogen storage and release device.
  • the micro-hollow ball 2 shown in FIG. 1 has a completely closed
  • Wall 20 which, as shown, here four sites with a hydrogen-sensitive catalyst 21, such as platinum coated.
  • a hydrogen-sensitive catalyst 21 such as platinum coated.
  • H 2 hydrogen gas
  • hp high pressure
  • the storage density of hydrogen is about 10 wt .-%. It is well known that at a lower pressure the gravimetric storage density decreases and the volumetric storage density increases due to the smaller wall thickness of the glass spheres. It follows that each hollow sphere has an optimized storage pressure.
  • micro-hollow spheres 2 located in a matrix Mx of surrounding H 2 O are not, as hitherto customary, by heating from the outside to the higher, for a release of the contained in the balls
  • Hydrogen H 2 is made permeable to the same, but in that the Catalytic converter 21 for a local catalytic reaction between the matrix Mx surrounding the micro-hollow spheres 2 and an externally supplied hydrogen-containing compound H 2 V, in particular sodium borohydride, NaBH 4 , and the local heat of reaction for the permeation ,
  • H 2 V in particular sodium borohydride, NaBH 4
  • substantially increasing the permeability of the micro-sphere wall 20 provides, at the same time in addition to the then emerging from the micro-hollow spheres 2 hydrogen, the hydrogen from the hydrogen-containing compound H 2 V comes, which ultimately total hydrogen then to a point of consumption is directed.
  • the system 1 for storing and releasing hydrogen shown in FIG. 2 comprises a first and a second storage container 3, 4, wherein in the first container 3 here liquid sodium borohydride, NaBH4, 30 and in the second storage container 4 a Wasser ⁇ / Hydrogen microballoon mixture 40 are located.
  • reaction end product 60 consisting of sodium boroxide and emptied micro-hollow spheres, is collected and can ultimately be recycled.
  • Controllable is the plant e.g. by means of a central control unit 7 connected to the above-mentioned pumps and valves.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Inorganic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • General Health & Medical Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Fuel Cell (AREA)
  • Hydrogen, Water And Hydrids (AREA)
  • Manufacturing Of Micro-Capsules (AREA)

Abstract

L'invention concerne un procédé et un dispositif pour stocker et libérer de l'hydrogène, procédé au cours duquel l'hydrogène est libéré de microsphères creuses remplies d'hydrogène. Ce procédé est caractérisé en ce qu'il consiste : à recouvrir la paroi des microsphères d'un catalyseur qui favorise la libération d'hydrogène, et à stocker les microsphères dans une matrice aqueuse; à stocker de manière séparée un hydrure, en particulier du borohydrure de sodium; et, en cas de besoin, à combiner le mélange eau/microsphères creuses remplies d'hydrogène et l'hydrure, en particulier le borohydrure de sodium, la réaction hydrure + eau = hydrogène + oxyde de l'hydrure ayant lieu sous l'action du catalyseur et générant de l'hydrogène et de la chaleur, ce qui rend les parois des microsphères creuses perméables à l'hydrogène et entraîne la libération et l'acheminment ultérieur de l'hydrogène contenu dans les microsphères; puis à évacuer et recycler le produit réactionnel final.
EP07784619A 2006-08-14 2007-08-14 Procédé et dispositif pour stocker et libérer de l'hydrogène Withdrawn EP2051931A2 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
AT0136506A AT503701B1 (de) 2006-08-14 2006-08-14 Verfahren zum speichern und gezielten freisetzen von wasserstoff
PCT/AT2007/000390 WO2008019414A2 (fr) 2006-08-14 2007-08-14 Procédé et dispositif pour stocker et libérer de l'hydrogène

Publications (1)

Publication Number Publication Date
EP2051931A2 true EP2051931A2 (fr) 2009-04-29

Family

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Family Applications (1)

Application Number Title Priority Date Filing Date
EP07784619A Withdrawn EP2051931A2 (fr) 2006-08-14 2007-08-14 Procédé et dispositif pour stocker et libérer de l'hydrogène

Country Status (3)

Country Link
EP (1) EP2051931A2 (fr)
AT (1) AT503701B1 (fr)
WO (1) WO2008019414A2 (fr)

Families Citing this family (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2435282B1 (fr) * 2009-05-27 2018-11-28 Månbas Alpha AB Manipulation de combustibles gazeux
SG2013022967A (en) 2013-03-25 2014-10-30 Horizon Energy Systems Pte Ltd Method and generator for hydrogen production

Family Cites Families (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4211537A (en) * 1978-07-24 1980-07-08 Teitel Robert J Hydrogen supply method
US4302217A (en) * 1978-07-24 1981-11-24 Teitel Robert J Hydrogen supply system
US4328768A (en) * 1980-07-24 1982-05-11 General Motors Corporation Hydrogen fuel storage and delivery system
AU2209197A (en) * 1996-11-13 1998-06-03 Minnesota Mining And Manufacturing Company Storage and delivery of pressurized gases in microbubbles
US6746496B1 (en) * 2002-01-15 2004-06-08 Sandia Corporation Compact solid source of hydrogen gas
US6866836B2 (en) * 2002-09-13 2005-03-15 General Motors Corporation Method of generating hydrogen from borohydrides and water
WO2004027901A2 (fr) * 2002-09-17 2004-04-01 Diffusion Science, Inc. Generation, stockage et reaction electrochimiques d'hydrogene et d'oxygene

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
See references of WO2008019414A2 *

Also Published As

Publication number Publication date
AT503701A4 (de) 2007-12-15
WO2008019414A2 (fr) 2008-02-21
AT503701B1 (de) 2007-12-15
WO2008019414A3 (fr) 2008-10-16

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