WO2007072470A1 - Appareil et cartouche pour le stockage d'hydrogene gazeux comprime et systeme permettant le remplissage de la cartouche - Google Patents

Appareil et cartouche pour le stockage d'hydrogene gazeux comprime et systeme permettant le remplissage de la cartouche Download PDF

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Publication number
WO2007072470A1
WO2007072470A1 PCT/IL2006/001082 IL2006001082W WO2007072470A1 WO 2007072470 A1 WO2007072470 A1 WO 2007072470A1 IL 2006001082 W IL2006001082 W IL 2006001082W WO 2007072470 A1 WO2007072470 A1 WO 2007072470A1
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WO
WIPO (PCT)
Prior art keywords
hydrogen
cartridge
microcylinders
chamber
controllable
Prior art date
Application number
PCT/IL2006/001082
Other languages
English (en)
Inventor
Valery G. Gnedenko
Igor V. Goryachev
Nikolay Zhevago
Original Assignee
C. En. Limited
Stern, Moshe
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 C. En. Limited, Stern, Moshe filed Critical C. En. Limited
Publication of WO2007072470A1 publication Critical patent/WO2007072470A1/fr

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    • 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
    • F17C13/00—Details of vessels or of the filling or discharging of vessels
    • F17C13/12—Arrangements or mounting of devices for preventing or minimising the effect of explosion ; Other safety measures
    • F17C13/123—Arrangements or mounting of devices for preventing or minimising the effect of explosion ; Other safety measures for gas bottles, cylinders or reservoirs for tank vehicles or for railway tank wagons
    • 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
    • F17C1/00—Pressure vessels, e.g. gas cylinder, gas tank, replaceable cartridge
    • 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
    • F17C13/00—Details of vessels or of the filling or discharging of vessels
    • F17C13/02—Special adaptations of indicating, measuring, or monitoring equipment
    • F17C13/025—Special adaptations of indicating, measuring, or monitoring equipment having the pressure as the parameter
    • 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
    • F17C13/00—Details of vessels or of the filling or discharging of vessels
    • F17C13/02—Special adaptations of indicating, measuring, or monitoring equipment
    • F17C13/026—Special adaptations of indicating, measuring, or monitoring equipment having the temperature as the parameter
    • 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
    • F17C13/00—Details of vessels or of the filling or discharging of vessels
    • F17C13/04—Arrangement or mounting of valves
    • 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
    • F17C5/00—Methods or apparatus for filling containers with liquefied, solidified, or compressed gases under pressures
    • F17C5/06—Methods or apparatus for filling containers with liquefied, solidified, or compressed gases under pressures for filling with compressed gases
    • 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
    • F17C7/00—Methods or apparatus for discharging liquefied, solidified, or compressed gases from pressure vessels, not covered by another subclass
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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    • F17C2201/05—Size
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    • 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
    • F17C2201/00—Vessel construction, in particular geometry, arrangement or size
    • F17C2201/05—Size
    • F17C2201/058—Size portable (<30 l)
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    • 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
    • F17C2203/00—Vessel construction, in particular walls or details thereof
    • F17C2203/06—Materials for walls or layers thereof; Properties or structures of walls or their materials
    • F17C2203/0602—Wall structures; Special features thereof
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    • F17C2203/0617—Single wall with one layer
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    • 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
    • F17C2203/00—Vessel construction, in particular walls or details thereof
    • F17C2203/06—Materials for walls or layers thereof; Properties or structures of walls or their materials
    • F17C2203/0602—Wall structures; Special features thereof
    • F17C2203/0612—Wall structures
    • F17C2203/0626—Multiple walls
    • F17C2203/0629—Two walls
    • 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
    • F17C2203/00—Vessel construction, in particular walls or details thereof
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    • F17C2203/00—Vessel construction, in particular walls or details thereof
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    • F17C2270/0184—Fuel cells
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    • F17C2270/00—Applications
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    • F17C2270/0186—Applications for fluid transport or storage in the air or in space
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    • F17C2270/00—Applications
    • F17C2270/05—Applications for industrial use
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
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    • 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
    • F17C2270/00—Applications
    • F17C2270/07—Applications for household use
    • F17C2270/0763—Fuel cells
    • 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 generally to fuel storage, and in particular, to accumulation and storage of hydrogen gas.
  • Hydrogen is a very high energy density element and clean- burning fuel.
  • the energy density of hydrogen which is around 120 MJ/kg, is more than double that of most conventional fuels, e.g., natural gas: 43 MJ/kg and gasoline 44.4 MJ/kg.
  • Hydrogen can be combined with oxygen through combustion, or through fuel cell mediated oxidation/reduction reactions, to produce heat, or electrical power.
  • the primary product of this reaction is water, which is non-polluting and can be recycled to regenerate hydrogen and oxygen.
  • Hydrogen can be stored as a cryogenic liquid, as a compressed gas in a large vessel, or bound chemically in a compound such as a metal Hydride.
  • Compressed hydrogen storage is the most common method for hydrogen storage. Typically the pressure levels are in the order of 20 MPa - 70 MPa.
  • Today's storage vessels usually are manufactured in fiber composite materials design in order to reduce structural weight.
  • An internal shell is made of stainless steel or aluminum and is wrapped with glass and/or carbon fibers.
  • the tank designs are also known which are made completely from plastic materials. Nevertheless, most compressed gaseous storage tanks are relatively large and heavy.
  • existing accumulation techniques with compressed gaseous hydrogen in tanks provide a relatively low hydrogen weight content (the ratio of the weight of hydrogen in accumulator to the weight of accumulator), i.e., less than 10 weight %, and there are certain restrictions for further growth of this parameter along with low explosion protection.
  • the storage of gaseous hydrogen in metal hydrides makes use of depositing hydrogen in metal alloys.
  • the hydrogen accumulation and storage techniques are relatively explosion-proof, because hydrogen features no excess pressure.
  • Disadvantages of metal hydride storage are that depending on the type of metal alloy, more or less elevated temperatures are needed to set hydrogen free again, and the low mass related storage density. Usually, the weight content of hydrogen is less than 4.5%.
  • also storage in other materials can be achieved by physical sorption. For example, storage of hydrogen in carbon nano-fibers is known. However, due to the weaker bonding of hydrogen in these solids the storage temperatures have to be lower than those for storage as metal hydrides.
  • the microsphere permeability to hydrogen will increase. Hydrogen can diffuse into the hollow cores of the microspheres through the thin glass walls at practical rates at temperatures between 100 0 C and 400 0 C. This provides the ability to fill the microspheres with gas by placing the microspheres in high-temperature and high pressure environments. Once cooled, the microspheres lock the hydrogen inside since the diffusion rate is drastically lower at room temperature. A subsequent increase in temperature will increase the diffusion rate. Thus, the hydrogen trapped in the microspheres can be released by subsequently increasing the temperature.
  • U.S. Pat. No. 4,328,768 describes a fuel storage and delivery system wherein hollow microspheres filled with hydrogen gas are stored in a fuel storage chamber at pressures of 400 atm. From the fuel storage chamber the microspheres are directed through a heated delivery chamber wherein hydrogen gas is freed by diffusion and delivered to an engine, after which the substantially emptied microspheres are delivered to a second storage chamber. The substantially emptied microspheres are removed by mechanical means, such as a pump, to a storage chamber from which they can be removed for refilling.
  • the present invention partially eliminates disadvantages of the prior art techniques and provides a novel apparatus for storage of compressed hydrogen gas including one or more novel cartridges containing hydrogen gas, a hydrogen liberating tool, and a control system configured for controlling operation of the apparatus.
  • the apparatus comprises a sealed housing having an outlet pipe coupled to the housing and equipped with a controllable discharge valve.
  • the sealed housing defines a chamber that includes the cartridge comprising a plurality of cylindrical voids containing said compressed hydrogen gas.
  • the cartridge can be either expendable (i.e., disposable) or rechargeable.
  • the hydrogen liberating tool is configured for controllable liberating the hydrogen gas from the cartridge into a volume of the chamber that is not occupied by the cartridge.
  • the control system is operatively coupled to the controllable discharge valve and the hydrogen liberating tool, and configured for controlling operation thereof.
  • the housing can include a detachable cover adapted to open and seal the housing.
  • the pressure of the hydrogen stored within the cylindrical voids can be higher than 1000 ami.
  • the pressure of the hydrogen accumulated within the volume of the chamber that is not occupied by the cartridge is in the range of 1 atm to 10 arm.
  • the control system includes a pressure sensor configured for producing a pressure sensor signal representative of the hydrogen gas pressure in the chamber.
  • the control system includes a flow meter configured for producing a gas flow sensor signal representative of the flow of the hydrogen gas pressure in the outlet pipe.
  • the control system also includes a controller operatively coupled to the pressure sensor and the flow meter. Accordingly, the control system is responsive to the pressure sensor signal and the gas flow sensor signal.
  • the controller is capable of generating control signals for controlling the operation of the hydrogen liberating tool and the discharge valve.
  • the apparatus can further include at least one safety valve that can be automatically open when pressure in the chamber reaches a dangerous level.
  • the cartridge includes a case and an assembly structure formed of plurality of closely packed hollow microcylinders arranged in the case.
  • the microcylinders have sealed ends, thereby they define the aforementioned cylindrical voids.
  • the microcylinders are made of material having relatively small hydrogen permeability at the temperatures below 60 0 C and more than 10 times higher permeability at the temperatures above 200 0 C.
  • a ratio of the tensile strength to the density of the material of the microcylinders can be greater than 1700 MPa-cm 3 /g.
  • the external diameter of the microcylinders can be in the range of 1 micrometer to 5000 micrometers.
  • a ratio of the wall thickness to the external diameter of the microcylinders can be in the range of 0.01 to 0.2.
  • the external diameter of the microcylinders can be reduced from a center of the assembly structure towards edges of the structure.
  • the wall thickness of the microcylinders can be increased from the center of the assembly structure towards the edges of the structure. Thickness of the case wall can be at least 10 times greater than the thickness of the microcylinder walls.
  • the hydrogen liberating tool includes an electrically heating element arranged within the cartridge, and a controllable power source coupled to the control system and configured for controllable powering the electrically heating element, whereby to controllably vary a temperature of the microcylinders.
  • the neighboring microcylinders can abut on one another at their walls, thereby forming empty inter-cylinder spaces along the microcylinders.
  • the electrically heating element can include a wire woven throughout the assembly structure of the plurality of closely packed hollow microcylinders such that folded segments of the wire are located in said inter-cylinder spaces. This allows a controllable changing of the temperature of the microcylinders and provides a controllable liberating of the hydrogen stored within the microcylinders into the inter-cylinder spaces and the other volume of the case that is not occupied by the microcylinders.
  • the cartridge can be equipped with at least one temperature sensor arranged in the inter-cylinder spaces.
  • the temperature sensor can be configured for measuring temperature of the microcylinders and producing a temperature sensor signal indicative of the temperature.
  • the control system is coupled to the temperature sensor and responsive to the temperature sensor signal for providing control of the electrically heating element, thereby to avoid overheating and damage of the cartridge.
  • the cartridge includes a monolithic block having a plurality of cylindrical cavities formed therein. Ends of the cylindrical cavities distal to the hydrogen liberating tool are sealed, whereas opposite ends of the cylindrical cavities (proximate to the hydrogen liberating tool) are covered with a hydrogen diffuser plate.
  • the cylindrical cavities define the aforementioned cylindrical voids.
  • the hydrogen diffuser plate can be made of a material characterized by photo-enhanced hydrogen diffusion.
  • the hydrogen diffuser plate can include a highly permeable to hydrogen substrate covered by a layer made of the material characterized by photo-enhanced hydrogen diffusion.
  • the hydrogen liberating tool includes a controllable radiation source operating in a predetermined radiation frequency range.
  • the controllable radiation source is coupled to the control system adapted to control the operation of the radiation source, thereby providing photo-enhanced diffusion of hydrogen through the hydrogen diffuser plate when it is illuminated by said controllable radiation source.
  • the control of the operation of the radiation source can be carried out by varying the intensity of the applied radiation.
  • the control of the operation of the radiation source can be carried out by turning the source on and off with a predetermined periodicity.
  • the hydrogen diffuser plate includes a layer of impermeable to hydrogen dielectric material perforated with a plurality of small holes plugged with stoppers that seal the holes. The density of the holes is such that at least one sealed opening is formed for each cylindrical cavity. According to this embodiment, a coefficient of thermal expansion of the layer is higher than the coefficient of thermal expansion of the stoppers.
  • the hydrogen liberating tool includes an electrically heating element.
  • the hydrogen liberating tool can include a heating layer made of conductive permeable to hydrogen material placed on the hydrogen diffuser plate and coupled to the controllable power source.
  • the cartridge includes an assembly structure formed of plurality of bound hollow microcylinders having both microcylinder ends sealed.
  • the hydrogen liberating tool can include an electric drive arranged in the housing.
  • hydrogen liberating tool includes an opener mounted on a shaft of the electric drive and configured for gradual destroying the microcylinder ends proximal to the liberating tool.
  • a direction of the shaft coincides with the direction of the cylinders, whereas the direction of the knife's blade is perpendicular to the direction of the shaft.
  • the electric drive includes an electric motor operatively coupled to the control system for providing controllable rotation of the shaft.
  • the apparatus and the control system can also be configured for providing controllable longitudinal motion of the shaft. For example, all the microcylinder ends proximal to the liberating tool can be destroyed during one total revolution of the shaft.
  • the cartridge includes a monolithic block having a plurality of cylindrical cavities formed therein having sealed ends and filled with hydrogen gas.
  • the hydrogen liberating tool can include an electric drive arranged in the housing, and an opener mounted on a shaft of the electric drive.
  • the opener is configured for gradual destroying the ends of the cavities proximal to the said hydrogen liberating tool, thereby providing liberation of the hydrogen gas gradually.
  • the electric drive can include an electric motor operatively coupled to the control system for providing controllable rotation of the shaft.
  • the apparatus and the control system can also be configured for providing controllable longitudinal motion of the shaft.
  • the apparatus according to the present invention is of durable and reliable construction. Moreover, the apparatus according to the present invention may have a low manufacturing cost.
  • a system for filling a cartridge having a plurality of cylindrical voids adapted for storing hydrogen gas includes an autoclave having a housing defining a chamber configured for holding the cartridge.
  • the system also includes an activation tool configured for operating an activation element providing hydrogen gas penetration into the cylindrical voids.
  • the system can include a controllable vacuum pump communicating with the chamber of the autoclave through a manifold equipped with a pump valve.
  • the controllable vacuum pump can be a roughing-down pump adapted to vacuumize the chamber up to the pressure of about 10 "3 - 10 ⁇ 2 torrs.
  • the system can also include a controllable evacuating unit that communicates with the chamber of the autoclave through the manifold equipped with an evacuation valve.
  • the system can also include a controllable blowing unit communicating with the chamber through manifold equipped with a blower valve and configured for blowing cooled hydrogen gas through the chamber.
  • the system also includes a controllable compressing unit communicating with the chamber through the manifold coupled to a vessel containing pure hydrogen gas used for the filling of the cartridge, and equipped with a compressor valve.
  • the system also includes a control unit coupled to at least one device selected from the activation element, the pump valve, the vacuum pump, the evacuating unit, the blowing unit, the compressing unit, the evacuation valve, the blower valve, the compressor valve, and configured for controlling operation thereof.
  • the housing is made of material that is capable to withstand the pressure values exceeding the pressure of the hydrogen gas maintained in said cylindrical voids of the cartridge after the filling.
  • the cartridge includes a case and an assembly structure formed of plurality of closely packed hollow microcylinders arranged in the case.
  • the microcylinders have sealed ends, thereby defining the aforementioned cylindrical voids.
  • the activation element includes a controllable electrically heating element arranged within the cartridge.
  • the electrically heating element can include an electrically conductive wire woven throughout the assembly structure of the microcylinders such that folded segments of the wire are located in inter-cylinder spaces.
  • the cartridge includes a monolithic block having a plurality of cylindrical cavities formed therein. Ends of the cylindrical cavities distal to the activation tool are sealed, whereas opposite ends of the cylindrical cavities proximate to the activation tool are covered with a hydrogen diffuser plate, thereby defining the aforementioned cylindrical voids.
  • the activation element can include a controllable radiation source configured to provide photo- enhanced diffusion of hydrogen through the hydrogen diffuser plate when the plate is illuminated by radiation of a predetermined frequency range.
  • the activation element can include a heating layer made of conductive permeable to hydrogen material placed on the hydrogen diffuser plate.
  • the system can also comprise a pressure sensor operable for producing a gas pressure sensor signal indicative of the pressure in the chamber.
  • the pressure sensor is coupled to the control unit which is responsive to the gas pressure sensor signal and capable of generating a control signal to at least one aforementioned system component for controlling thereof.
  • the system can also comprise a temperature sensor operable for producing a gas temperature sensor signal indicative of the temperature within the chamber.
  • the temperature sensor is coupled to the control unit which is responsive to the temperature sensor signals and capable of generating a control signal to aforementioned system component for controlling thereof.
  • the method comprises placing the cartridge into a chamber; vacuumizing the chamber to a predetermined pressure; preparing the cartridge in order to let the hydrogen gas diffuse into the cylindrical voids; and controlled compressing the hydrogen gas in the chamber over a predetermined compression time interval while maintaining the step of preparing the cartridge operating until the pressure in the chamber reaches a predetermined pressure value, thereby providing the hydrogen gas diffusion into the cylindrical voids.
  • the predetermined pressure value is up to about 3000 atm.
  • the predetermined compression time interval is in the range of several minutes to several hours.
  • the cartridge includes a case and an assembly structure formed of plurality of closely packed hollow microcylinders arranged in the case.
  • the microcylinders have sealed ends, thereby defining the aforementioned cylindrical voids.
  • the step of preparing of the cartridge includes heating the microcylinders to a predetermined temperature.
  • the predetermined temperature can be in the range of about 300 0 C- 500 0 C.
  • the cartridge includes a monolithic block having a plurality of cylindrical cavities formed therein.
  • the cylindrical cavities are sealed at one end and covered with a hydrogen diffuser plate at another end.
  • the step of preparing of the cartridge includes illuminating said hydrogen diffuser plate by radiation of a predetermined frequency range, thereby to provide photo-enhanced diffusion of hydrogen therethrough.
  • the step of preparing of the cartridge can include heating the hydrogen diffuser plate to a predetermined temperature.
  • the method can further comprise the steps of terminating the preparing of the cartridge, and the controlled hydrogen gas compressing; depressurizing the chamber; and blowing cooled hydrogen gas through the chamber.
  • the method can further comprise the steps of: terminating the preparing of the cartridge, while maintaining the hydrogen gas compressing step to operate, thereby to keep the pressure in the chamber at the maximal value over the time interval until the cartridge is returned to the condition of small hydrogen permeability; and depressurizing the chamber.
  • Fig. 1 is a schematic cross-sectional view of an apparatus for storage of hydrogen gas is illustrated
  • Fig. 2A is a cross-sectional schematic view of the apparatus of Fig. 1 including a hydrogen storage cartridge and a hydrogen liberating tool, according to one embodiment of the present invention
  • Fig. 2B is a top cross-sectional schematic view of the apparatus of Fig. 2A taken along the line A-A therein;
  • Fig. 3 A is a schematic view of the apparatus of Fig. 1 having the hydrogen storage cartridge and the hydrogen liberating tool according to another embodiment of the present invention
  • Fig. 3B is a top cross-sectional schematic view of the apparatus of Fig. 3A taken along the line B-B therein;
  • Fig. 4 is schematic view of the apparatus of Fig. 1 having the hydrogen storage cartridge and the hydrogen liberating tool according to still another embodiment of the present invention
  • Fig. 5 shows schematically an example of a perforated layer of the hydrogen diffuser plate, according to this embodiment of the invention
  • Fig. 6 is a schematic view of me apparatus of Fig. 1 having the hydrogen storage cartridge and the hydrogen liberating tool according to yet another embodiment of the present invention
  • Fig. 7 is a schematic cross-sectional view of a system for filling the cartridge of the present invention with hydrogen gas;
  • Fig. 8 shows an exemplary packaging of an assembly of microcylinders in the hydrogen storage cartridge
  • Fig. 9 shows an exemplary group of microcylinders having a hexagonal cross- section shape.
  • the hydrogen storage apparatus 10 comprises a housing 11 having a detachable cover 12 adapted to open and seal the housing 11.
  • the sealed housing 11 defines a chamber 13 that includes a cartridge (module) 14 mounted in the chamber 13 with the help of fasteners (not shown).
  • the cartridge 14 includes a plurality of cylindrical voids (not shown in Fig. 1) containing compressed hydrogen gas.
  • the cartridge 14 can be either expendable or rechargeable.
  • the cartridge 14 can be inserted into the chamber 13 and removed therefrom through an opening (not shown) that is sealed by the detachable cover 12.
  • the apparatus 10 also includes a hydrogen liberating tool diagrammatically represented by a box 15, and a control system 16 operatively coupled to the hydrogen liberating tool 15 and configured for controlling operation thereof.
  • the hydrogen liberating tool 15 is configured for controllable liberating hydrogen gas from the cartridge 14 in which the hydrogen is stored at very high pressures into a volume of the chamber 13 that is not occupied by the cartridge 14 and in which the hydrogen is stored at a moderate pressure.
  • the pressure of the hydrogen stored within the cartridge 14 can be higher than 1000 atm (e.g., in the range of 1000 atm - 3000 atm), whereas the pressure of the hydrogen within the unoccupied volume of the chamber 13 can be in the range of 1 atm- 10 atm.
  • control system 16 For measuring pressure of the hydrogen within the unoccupied volume of the chamber 13 the control system 16 includes a pressure sensor 161 that is operable for producing a gas pressure sensor signal.
  • the pressure sensor 161 is coupled to a controller 162 of the control system 16 which is, inter alia, responsive to the gas pressure sensor signal and capable of generating a control signal to the hydrogen liberating tool 15 for controllable liberation of the compressed hydrogen gas from the cartridge 14.
  • Shape of the housing 11 can, for example, be tubular. However, it should be understood that generally, any desired shape of the housing 11 can be used.
  • the housing 11 can be constructed of a suitable metal, plastic or composite material with thickness of the walls appropriate to withstand the strain on the walls caused by the gas pressure inside the housing 11.
  • the apparatus 10 also includes an outlet pipe 17 coupled to the housing 11.
  • the control system 16 also includes a flow meter 163 and a discharge valve 164 arranged in the outlet pipe 17 and coupled to the controller 162 for controllable discharge of the gaseous hydrogen from the chamber 13.
  • the flow of the hydrogen gas within the outlet pipe 17 is measured by the flow meter 163 that is operable for producing a gas flow sensor signal.
  • the flow meter 163 is coupled to the controller 162 which is, inter alia, responsive to the gas flow sensor signal and capable of generating a valve control signal for controlling the operation of the discharge valve 164.
  • the hydrogen discharged thereby can be used as a fuel or as a raw material in reactions desired by a user.
  • the apparatus 10 can also include one or several safety valves 18 that can automatically open when pressure in the chamber 13 reaches a dangerous level.
  • the structure of the hydrogen storage cartridge 14 and the hydrogen liberating tool 15 can have various configurations.
  • Figs. 2A and 2B a schematic view of the apparatus of Fig. 1 in which the rechargeable cartridge 14 for hydrogen storage and the hydrogen liberating tool 15 are illustrated according to one embodiment of the present invention.
  • the cartridge 14 includes a case 141 and an assembly structure 142 of micro-containers located in the case 141.
  • the assembly structure 142 of the micro-containers includes a plurality of closely packed hollow microcylinders (microtubes) 21.
  • Ends 22a and 22b of the microcylinders 21 are sealed, e.g., capped on the ends by semi-spheres with comparable wall thickness, thereby defining the voids in which the compressed hydrogen gas is contained.
  • the hollow microcylinders 21 themselves or at least one of the sealed ends 22a and 22b are made of a material that is at least partially permeable to hydrogen, to allow hydrogen molecules to diffuse therethrough.
  • the hollow microcylinders 21 are made of material having relatively small hydrogen permeability at temperatures below 60 0 C and high permeability (more than 10 times higher) at temperatures above 200 0 C.
  • the materials having high tensile strength ⁇ at low density p are selected for the microcylinders 21.
  • the materials that meet the condition ⁇ /p ⁇ 1700 MPa-cm 3 /g are suitable for the microcylinders 21.
  • the materials suitable for the microcylinders 21 include, but are not limited to, MgAlSi glasses (e.g., S-2 Glass , R glass available from Saint-Gobain Vetrotex Textiles, T Glass available from Nitto Boseki Co., Ltd. (Nittobo)), fused quartz, polymers (e.g., Kevlar , Twaron ), etc.
  • the hollow microcylinders 21 can have any desired length.
  • the external diameter d of the microcylinders 21 can be in the range of about 1 micrometer to 1 millimeter.
  • the ratio of the wall thickness to the external diameter is in the range of 0.01 to 0.2, depending on ⁇ » and ⁇ .
  • the external diameter d and wall thickness h of the microcylinders located in the inner layers (i.e., in the bulk) of the assembly structure 142 and the peripheral microcylinders can be different, hi particular, the external diameter of the microcylinders 21 can be reduced from a center of the assembly structure towards edges of the structure.
  • the wall thickness h of the microcylinders can be increased from the center of the assembly structure towards the edges of the structure.
  • the assembly 142 of the microcylinders 21 is enveloped by the case 141.
  • the inner surface of the case wall can be bound to the peripheral microcylinders of the assembly 142.
  • the case 141 can be constructed of any suitable metal, plastic or composite material, and be of any desired shape and configuration having rigidity sufficient for manipulation of the cartridge for its insertion into and removing from the housing 11.
  • the case 141 and the microcylinders 21 are made of the same material. Thickness of the case wall can be 10-12 times greater than the thickness of the microcylinder walls.
  • the case 141 can have cylindrical shape, i.e., replicate the shape of the inner surface of the housing 11. Generally, the case 141 can have any desired shape.
  • the case 141 can be equipped with a carry handle 143 arranged to facilitate a user to insert, remove and/or carry the cartridge 14.
  • the microcylinders 21 in the assembly structure 142 are circular in their cross-section and closely (intimately) packed in the case 141, but they are not bound together.
  • the microcylinders 21 are bound together to form a rigid structure, hi this case, the microcylinders 21 can have any arbitrary form in their cross-section, e.g. hexagonal (see Fig. 8).
  • the microcylinders are made of glass, aramid or metal, they can be bound together, for example, by sintering.
  • an adhesive material such as glue, can also be used for binding the microcylinders.
  • the hydrogen liberating tool 15 includes an activation element, such as an electrically heating element 145 arranged within the cartridge 14 for activation of liberation (diffusion release) of the hydrogen gas stored within the microcylinders 21.
  • the electrically heating element 145 is powered by a controllable power source 151 arranged outside of the housing 11 and coupled to the control system 16. In operation, depending on the pressure of the hydrogen gas within the chamber 13 measured by the pressure sensor 19, the control system is, inter alia, adapted to control the operation of the power source 151.
  • the electrically heating element 145 powered by the controllable power source 151 can controllably vary the temperature within the cartridge 14, thereby providing a controllable liberating of the hydrogen stored within the microcylinders 21 into the inter-cylinder spaces 144 and the other volume of the case 141 that is not occupied by the microcylinders 21.
  • the hydrogen gas accumulated in the cartridge 14 will further diffuse through the case 141 into the volume of the chamber 13 that is not occupied by the cartridge 14.
  • the electrically heating element 145 includes a wire 146 woven throughout the assembly structure 142 such that folded segments 147 of the wire are located in the inter-cylinder spaces 144.
  • the wire segments 147 can be connected in series and represent one circuit.
  • the wire segments 147 can be grouped in several circuits.
  • the microcylinders 21 can be arranged (bundled) in groups.
  • Each group can include more than 2 microcylinders and have any desired cross- section shape, e.g. circular, oval, polygonal, etc.
  • the cross-section shape of each group is hexagonal (see Fig. 9), to provide the possibility of the closest packing of the groups.
  • the folded segments 147 of the wire can be located in the interphase between the neighboring groups.
  • electric voltage is applied across the circuit(s)
  • electric current passing therethrough is produced for heating the wire segments and consequently the microcylinders 21.
  • Ends 148 of the wire 146 are brought out to one part of a connector 149 arranged at the outer side of the case 141.
  • Another part of the connector 149 can be arranged within the housing 11 and coupled to the power source 151.
  • the connector 149 connects the wire 146 to the controllable power source 151.
  • the controllable power source 151 can be controlled in such a manner that the voltage applied across the circuit or number of the circuits powered by the power source 151 is increased when the pressure in the chamber 13 is lower than the required level, and vice versa, the voltage applied across the circuit or number of the circuits powered by the power source 151 is decreased when the pressure in the chamber 13 is higher than the required level.
  • the cartridge 14 can be equipped with one or several temperature sensors 152 arranged in the inter-cylinder spaces 144, and configured for measuring temperature of the microcylinders 21 and producing a temperature sensor signal indicative of the temperature.
  • the temperature sensors 152 are coupled to the control system 16 which is, inter alia, responsive to the temperature sensor signal and capable of providing a control of the electrically heating element 145 to avoid overheating and damage of the cartridge elements.
  • the cartridge 14 includes a monolithic block 31 having a plurality of cylindrical cavities 32 formed therein.
  • the material of the monolithic block 31 is impermeable to hydrogen.
  • Ends 33 of the cylindrical cavities 32 distal to the hydrogen liberating tool 15 are sealed.
  • Ends 34 of the cylindrical cavities 32 proximate to the hydrogen liberating tool 15 are covered with a hydrogen diffuser plate 35.
  • the cylindrical cavities 32 (sealed from the two ends) form the cylindrical voids of the invention in which hydrogen gas can be stored at very high pressure.
  • the hydrogen diffuser plate 35 features photo-enhanced hydrogen diffusion characteristics.
  • the hydrogen diffuser plate 35 is made of a material characterized by photo-enhanced hydrogen diffusion.
  • the hydrogen diffuser plate 35 includes a highly permeable to hydrogen substrate covered by a layer made of the material characterized by photo-enhanced hydrogen diffusion.
  • IR infrared
  • the materials that demonstrate great acceleration of the release rate of hydrogen through the hydrogen diffuser plate 35 owing the infrared (IR) radiation are known in the art (see, for example, a paper titled "Photo-Enhanced Hydrogen Outgassing of Glass," by D. B. Rapp and J. E. Shelby, published in J. Non-Cryst. Solids, 2004, V. 349, PP. 254-259).
  • doping commercially available borosilicate glasses with optically active elements e.g., Fe 3 O 4
  • the hydrogen liberating tool 15 includes an activation element, such as a controllable radiation source 36 providing photo-enhanced diffusion of hydrogen through the hydrogen diffuser plate 35 when the plate 35 is illuminated by the radiation of the predetermined frequency range.
  • an activation element such as a controllable radiation source 36 providing photo-enhanced diffusion of hydrogen through the hydrogen diffuser plate 35 when the plate 35 is illuminated by the radiation of the predetermined frequency range.
  • the controllable radiation source 36 can operate in various ranges of the electromagnetic scale.
  • the controllable radiation source 36 can be an infrared (IR) lamp.
  • the IR radiation causes the dopant to react, opening up the microscopic pores that occur naturally in the glass.
  • the hydrogen which is under high pressure inside the voids formed of the sealed cylindrical cavities 32, can diffuse through the pores opened in the hydrogen diffuser plate 35.
  • the release of the hydrogen from the cylindrical voids can be controlled by varying the intensity of the IR radiation and/or by simply turning the IR source on and off.
  • the radiation source 36 is controlled by the control system 16.
  • the control system is, inter alia, adapted to control the operation of the radiation source 36 by varying the intensity of the applied radiation and/or by turning the source on and off with a predetermined periodicity, thereby providing a controllable liberating of the hydrogen stored within the cylindrical cavities 32 into the volume of the chamber 13 that is not occupied by the cartridge 14. For example, when the pressure in the chamber is low, the intensity of the radiation can be increased, and vice versa.
  • FIG. 4 a schematic view of the apparatus of Fig. 1 in which the hydrogen storage cartridge 14 and the hydrogen liberating tool 15 are illustrated according to still another embodiment of the present invention.
  • the cartridge differs from the cartridge shown in Fig. 3A in the construction of the hydrogen diffuser plate that is indicated in Fig. 4 by a reference numeral 41.
  • the hydrogen diffuser plate 41 includes a layer 42 of impermeable to hydrogen dielectric material perforated with a plurality of small holes 43.
  • Fig. 5 shows schematically an example of the layer 42 of the hydrogen diffuser plate 41, according to this embodiment of the invention.
  • the density of the holes 43 is such that at least one opening must be formed for each cylindrical cavity (32 in Fig.
  • the sealed cylindrical cavities 32 form the cylindrical voids of the invention in which hydrogen gas can be stored at very high pressure.
  • the materials selected for the layer 42 and the stoppers 44 feature different coefficients of thermal expansion. Specifically, the coefficient of thermal expansion of the layers 42 is higher than the coefficient of thermal expansion of the stoppers 44.
  • the materials suitable for the layer 42 include, but are not limited to, borosilicate glass, quartz and some metals.
  • the materials suitable for the stoppers 44 include, but are not limited to, glasses of the titanium-silica family, anisotropic Invar Fe-Ni alloys and ZrW 2 O 3 , which have negative linear thermal expansion coefficient along the specific axis.
  • Such a construction of the holes and stoppers inside the holes forms thermophysical microvalves that can operate as follows.
  • the mismatch of the thermal expansion coefficients will result in the formation of the gap 46 between an inner surface of the holes 43 and edges of the stoppers 44.
  • the holes and the stoppers have a circular shape, an annular gap is formed.
  • the shape of the holes 43 and stoppers 44 is not bound by the circular shape.
  • suitable shapes include, but are not limited to, rectangular shape, polygonal shape, elliptical shape, etc.
  • the hydrogen liberating tool 15 includes an activation element, such as an electrically heating element 45 arranged in the proximity to the hydrogen diffuser plate 41.
  • the electrically heating element 45 can include a heating layer 451 made of conductive permeable to hydrogen material that is placed on the hydrogen diffuser plate 41 and coupled to the controllable power source 151.
  • the materials suitable for the heating layer 451 include, but are not limited to, porous graphite or Pd-Ni alloys.
  • the electrically heating element 45 is powered by the controllable power source 151 arranged outside of the housing 11 and coupled to the control system 16. In operation, depending on the pressure of the hydrogen gas within the chamber 13 measured by the pressure sensor 19, the control system is, inter alia, adapted to control the operation of the power source 151.
  • the electrically heating element 45 powered by the controllable power source 151 can controllably vary the temperature of the hydrogen diffuser plate 41. Specifically, when electric voltage produced by the power source 151 is applied across the heating layer 451, electric current passing therethrough is produced that generates heat for heating the hydrogen diffuser plate 41 arranged under the heating layer 451.
  • the micro-containers formed of a plurality of closely packed microcylinders and/or the cylindrical cavities in the monolithic block described above can be sealed.
  • the microcylinders can be closed by caps, for example, after being filled with hydrogen inside a high- pressure chamber, e.g., by applying melting temperature to the ends. Hydrogen release can be organized by one-by-one destroying of the caps, mechanically or by other means.
  • Fig. 6 a schematic view of the apparatus of Fig. 1 in which the hydrogen storage cartridge 14 and the hydrogen liberating tool 15 are illustrated, according to yet another embodiment of the present invention.
  • the cartridge 14 can include a monolithic block 31 having a plurality of cylindrical cavities (such as voids) 32 formed therein.
  • the material of the monolithic block 31 can be impermeable to hydrogen.
  • the ends 33 and 34 of the cylindrical cavities 32 can be sealed.
  • the cartridge 14 can include a plurality of hollow microcylinders having sealed ends, which are bound in an assembly structure and charged with the hydrogen gas.
  • the microcylinders can be tied with a fastener, e.g., girded with a fastening band.
  • the microcylinders can be welded together.
  • the ends of the cylindrical cavities proximate to the hydrogen liberating tool are protruded from the assembly structure.
  • the hydrogen liberating tool 15 includes an activation element, such as an electric drive 153 arranged in the housing 11 and an opener (e.g., knife) 154 mounted on a shaft 155 of the electric drive 153.
  • an activation element such as an electric drive 153 arranged in the housing 11 and an opener (e.g., knife) 154 mounted on a shaft 155 of the electric drive 153.
  • a direction of the shaft 155 coincides with the direction of the cylinders (or cylindrical cavities), whereas the direction of the knife's blade is perpendicular to the direction of the shaft 155.
  • the electric drive 154 includes an electric motor 156 that provides rotation of the shaft 155.
  • the electric motor 156 is mounted on the outer surface of the housing 11 at one of its ends.
  • the electric motor 156 is operatively coupled to the control system 16.
  • the control system 16 is, inter alia, responsive to the gas pressure sensor signal generated by the pressure sensor 161, and is capable of generating a motor control signal to the electric motor 156 for control of angular velocity of rotation of the knife 154. It should be understood that if required by the configuration of the cylinders in the cartridge 14, the control system 16 can also control feed of knife 154 by providing longitudinal motion of the shaft 155.
  • Hydrogen liberation can be organized in a gradual manner, e.g., by one-by-one cutting the ends 34 with the knife 154.
  • the electric motor 156 can be controlled in such a manner that the velocity of rotation of the knife 154 is increased when the pressure in the chamber 13 is lower than the required level, and vice versa, the velocity is decreased when the pressure in the chamber 13 is higher than the required level.
  • the electric drive 154 can be configured such that during the total destruction of the ends 34, the shaft maintains one total revolution.
  • a method of filling the cartridge 14 with hydrogen gas is provided.
  • hydrogen filling into the cylindrical voids occurs by permeation (diffusion) through walls of the microcylinders (21 in Fig. 2A) or through the hydrogen diffuser plate (35 in Fig. 3A).
  • the overall rate of hydrogen transport through the wall/plate depends on the temperature, the thickness of the wall or diffuser plate, the pressure difference and the exchange surface area available.
  • the system 70 includes an autoclave 71 having a housing 711 made of material that is capable to withstand very high pressure, hi particular, the housing 711 should be capable of withstanding the pressure values exceeding the pressure of the hydrogen gas maintained in the cylindrical voids of the cartridge after the filling.
  • the materials suitable for the housing 711 include, but are not limited to, composite materials containing carbon, quartz and/or aramid filaments.
  • the housing 711 defines a chamber 712 configured for holding the cartridge 14 that is inserted therein for filling with hydrogen. After the insertion, the housing 711 is sealed, for example, by means of a cover 713 that covers an opening (not shown) at one of the housing ends through which the cartridge is inserted.
  • the autoclave 71 also includes an activation tool 714 configured for operating activation elements (not shown) that provide the hydrogen gas to penetrate into the cylindrical voids of the cartridge.
  • the arrangement and configuration of the activation elements are determined by the type of the cartridge 14.
  • the activation element can include the controllable electrically heating element arranged within the cartridge.
  • the electrically heating element can be powered by a controllable power source (not shown) arranged outside of the autoclave 71.
  • the electrically heating element includes a wire woven throughout the assembly structure of the microcylinders 21 such that folded segments of the wire are located in the inter-cylinder spaces.
  • the activation element can include the controllable radiation source that can provide photo-enhanced diffusion of hydrogen through the hydrogen diffuser plate (35 in Fig. 3A) when the plate 35 is illuminated by the radiation of the predetermined frequency range.
  • the activation element can include the electrically heating element arranged in the proximity to the hydrogen diffuser plate (41 in Fig. 4).
  • the electrically heating element can include a heating layer (451 in Fig. 4) made of conductive permeable to hydrogen material that is placed on the hydrogen diffuser plate 41 and coupled to the controllable power source (not shown).
  • the activation element can include the electrically heating element configured for controllable varying the temperature of the ends of either the cylindrical cavities proximate to the activation element or the plurality of hollow microcylinders. It should be understood that these ends can be sealed, e.g., capped by semi-spheres made of the material having relatively small hydrogen permeability at temperatures below 60 0 C and high permeability (more than 10 times higher) at temperatures above 200 0 C. In the latter case, when the cartridge includes the assembly structure of hollow microcylinders, the walls of the microcylinders as well can be made of such a material.
  • the system 70 also includes a controllable vacuum pump 72, e,g., a roughing- down pump, communicating with the chamber 712 of the autoclave 71 through a branch 731 of a manifold 73 equipped with a pump valve 721.
  • the controllable vacuum pump 72 is configured to vacuumize (rough-down) the chamber 712 up to the pressure of about 10 "3 torrs - 10 '2 torrs.
  • the system 70 can also include a controllable evacuating unit 74 that communicates with the chamber 712 of the autoclave 71 through a branch 732 of the manifold 73 that is equipped with an evacuation valve 741.
  • the evacuating unit 74 can include a buffer vessel (not shown) and operate under support of the controllable vacuum pump 72.
  • the system 70 further includes a controllable blowing unit 75 communicating with the chamber 712 through a branch 733 of the manifold 73 that is equipped with a blower valve 751.
  • the controllable blowing unit 75 is configured for blowing cooled hydrogen gas through the chamber 713.
  • the system 70 further includes a controllable compressing unit 76 communicating with the chamber 712 through a branch 734 of the manifold 73 that is coupled to a vessel 77 containing pure hydrogen gas used for the filling of the cartridge 14, and equipped with a compressor valve 761.
  • the controllable compressing unit 76 is configured for smooth or step changes of the pressure of the hydrogen gas fed into the chamber 712, in accordance with a predetermined algorithm determined by the type of the cartridge 14.
  • the system 70 also includes a control unit 78 coupled to the activation element(s) of the activation tool 714, the vacuum pump 72, the evacuating unit 74, the blowing unit 75, the compressing unit 76, the valves 721, 741, 751 and 761, and configured for controlling the operation these elements of the system 70.
  • the activation element includes a heating element (see, for example, Figs. 2A and 4)
  • the activation element can be coupled to the control unit 78 and the corresponding electric power source (not shown) through a connector 715 arranged in the housing 711 of the autoclave 71.
  • the system 70 For measuring pressure of the hydrogen gas in the chamber 712, the system 70 includes a pressure sensor 781 that is operable for producing a gas pressure sensor signal indicative of the pressure in the chamber 712.
  • the system 70 can also include a temperature sensor 782 that is operable for producing a gas temperature sensor signal indicative of the temperature within the chamber 712.
  • the pressure sensor 781 and the temperature sensor 782 are coupled to the control unit 78 which is, inter alia, responsive to the gas pressure and temperature sensor signals and capable of generating control signals to all the controllable elements of the system for operating thereof.
  • the cartridge 14 to be filled with hydrogen is placed in the chamber 712 of the autoclave 71 that is then sealed with the cover 713.
  • the parts of the connector 715 are inserted one inside the other, thereby providing the coupling of the activation element to the control unit 78 and the electric power source.
  • Filling the cartridge 14 with high-pressure hydrogen gas can be a batch process that generally includes placing the cartridge into the chamber 712 of the autoclave 71; purging the chamber 712 in order to vacuumize it to a predetermined pressure; preparing the cartridge in order to let the hydrogen gas to diffuse into said cylindrical voids; and controlled compressing the hydrogen gas in the chamber over a predetermined compression time interval.
  • the autoclave 71 is purged by vacuumizing (roughing-down) up to the pressure of about 10 "3 - 10 ⁇ 2 torrs by the controllable vacuum pump 72 to remove air from the chamber 712 of the autoclave 71, thereby preparing the chamber to be fed with hydrogen gas.
  • the process of filling the cartridge 14 with hydrogen gas involves actuating the activating unit 714 over a required time interval that can include a predetermined period of preliminary preparation of the cartridge 14 to receive hydrogen, and then a predetermined compression period.
  • the actuating of the activating unit 714 can include heating the microcylinders (21 in Fig. 2A) or the hydrogen diffuser plate (41 in Fig. 4).
  • the cartridge 14 is heated to a temperature in the range of 300°G-500°C (depending on the material of the microcylinders), thereby preparing the cartridge 14 for letting the hydrogen gas to diffuse into the cylindrical voids.
  • the actuating of the activating unit 714 can include a controllable operating of the radiation source (36 in Fig. 3A).
  • the process includes actuating the compressing unit 76 that provides pure hydrogen gas from the vessel 77 to the chamber 712.
  • the pressure in the chamber 712 increases.
  • the activating unit 714 continues to operate, the cylindrical voids of the cartridge 14 can receive the hydrogen gas and the pressure in the cylindrical voids also increases.
  • the autoclave is maintained under this regime until the hydrogen gas pressure in the autoclave reaches a predetermined pressure value. For example, the pressure in the autoclave can reach the value of about 3000 atm.
  • the time needed to fill the cylindrical voids depends on many factors, such as the temperature level and the final filling pressure.
  • the compression interval can be in the range of several minutes to several hours.
  • the pressurization rate during filling procedure can be controlled such that the pressure difference between outer and inner cylindrical void pressure does not exceed the stress limit for the void to collapse.
  • the activating unit 714 and the compressing unit 76 can be both switched off, and the valve 761 is closed, hi turn, the chamber 712 is coupled to the evacuating unit 74 through the valve 741 for depressurization of the chamber 712.
  • the valve 741 is closed and the chamber 712 is coupled to the controllable blowing unit 75 for blowing cooled hydrogen gas through the chamber 713.
  • the cartridge is cooled down and transformed in the regime of storing the hydrogen gas accumulated therein during the compression time interval.
  • the filled cartridge can be removed from the autoclave 71 and utilized by a consumer.
  • the activating unit 714 is switched off, whereas the compressing unit 76 is still maintained operating, thereby to keep the pressure in the chamber at the maximal value over a certain time interval until the cartridge is returned to the condition of small hydrogen permeability.
  • the cartridge of the embodiments shown in Figs. 2A and 4 can be cooled down to the room temperature. It should be understood that this scenario prevents the release of hydrogen from the cartridge over the time interval when the activating unit 714 (facilitating diffusion of hydrogen into the cylindrical voids) is switched off. Then, the hydrogen pressure in the autoclave can be dropped, and the cartridge can be removed from the autoclave.

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  • Engineering & Computer Science (AREA)
  • Mechanical Engineering (AREA)
  • General Engineering & Computer Science (AREA)
  • Filling Or Discharging Of Gas Storage Vessels (AREA)

Abstract

L'invention concerne un appareil pour le stockage d'hydrogène gazeux comprimé. L'appareil contient un logement hermétique possédant un tuyau de sortie couplé au logement et équipé d'une vanne de refoulement pouvant être commandée. Le logement hermétique définit une chambre renfermant une cartouche comprenant une pluralité de vides cylindriques contenant ledit hydrogène gazeux comprimé. L'appareil comporte également un outil de libération d'hydrogène conçu pour libérer de façon contrôlée de l'hydrogène gazeux de la cartouche vers l'intérieur d'un volume de la chambre non occupé par la cartouche. L'appareil est commandé par un système de commande couplé de manière opérationnelle à la vanne de refoulement commandée et à l'outil de libération d'hydrogène, et conçu pour commander leur fonctionnement. Selon un autre aspect, elle concerne un système et un procédé de remplissage de la cartouche. Le remplissage consiste à dépressuriser une chambre dans laquelle la cartouche est placée, à préparer la cartouche afin de laisser l'hydrogène gazeux se diffuser dans les vides cylindriques et à comprimer de façon régulée le gaz hydrogène dans la chambre pendant un intervalle de temps de compression prédéterminé jusqu'à ce que la pression dans la chambre atteigne une valeur prédéterminée.
PCT/IL2006/001082 2005-12-22 2006-09-14 Appareil et cartouche pour le stockage d'hydrogene gazeux comprime et systeme permettant le remplissage de la cartouche WO2007072470A1 (fr)

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US75237905P 2005-12-22 2005-12-22
US60/752,379 2005-12-22

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Cited By (16)

* Cited by examiner, † Cited by third party
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WO2008042710A2 (fr) * 2006-09-29 2008-04-10 Praxair Technology, Inc. Système de distribution de gaz très pur à faible tension de vapeur
EP2062850A2 (fr) 2007-11-08 2009-05-27 C. EN. Limited Appareil de stockage et libération de gaz hydrogène comprimé dans des réseaux microcylindriques et système de remplissage de réseaux microcylindriques
WO2009090491A3 (fr) * 2007-11-30 2009-09-03 Honda Motor Co., Ltd. Systèmes de réchauffement pour dispositifs de stockage de gaz à haute pression
EP2163805A2 (fr) 2008-09-11 2010-03-17 C. En. Limited Appareil pour le stockage de gaz
DE102009016475A1 (de) 2008-04-01 2010-04-15 Deutsches Zentrum für Luft- und Raumfahrt e.V. Wasserstoffbereitstellungssystem und Verfahren zur Bereitstellung von Wasserstoff
WO2011080746A1 (fr) * 2010-01-04 2011-07-07 C. En. Limited Appareil de stockage d'hydrogène gazeux comprimé dans des batteries de micro-cylindres
CN101504112B (zh) * 2008-02-07 2011-08-24 林德股份公司 加氢燃料的方法
JP2012513572A (ja) * 2008-12-23 2012-06-14 エンサイト・エルエルシー ガス貯蔵システム
WO2013045043A1 (fr) * 2011-10-01 2013-04-04 Daimler Ag Dispositif destiné au stockage d'un combustible gazeux
DE102011087023A1 (de) 2011-11-24 2013-05-29 Helmholtz-Zentrum Berlin Für Materialien Und Energie Gmbh Verfahren und anordnung zur hochdruckspeicherung von wasserstoffgas
US8796600B2 (en) 2007-11-30 2014-08-05 Honda Motor Co., Ltd. Induction warming system for fiber composite gas storage cylinders
US9052063B2 (en) 2012-01-20 2015-06-09 L'Air Liquide Société Anonyme Pour L'Étude Device for storage of compressed gas, method of making the same, and method of using the same
WO2015019094A3 (fr) * 2013-08-08 2016-04-21 Intelligent Energy Limited Appareil et procédé de remplissage de gaz
CN105715942A (zh) * 2014-12-05 2016-06-29 刘建华 内置cng气瓶玻璃钢储罐
WO2017037429A3 (fr) * 2015-08-28 2017-04-27 Intelligent Energy Limited Appareil de stockage de vase de dewar
CN113915525A (zh) * 2021-10-29 2022-01-11 江苏氢枫能源装备有限公司 一种固态储氢氢气吸附与释放装置

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US20030192779A1 (en) * 2002-04-15 2003-10-16 Yaw-Chung Cheng Device for charging and activating hydrogen storage canister
WO2005028945A2 (fr) * 2003-09-19 2005-03-31 Prototech As Stockage de fluides pressurises
WO2006046248A1 (fr) * 2004-10-27 2006-05-04 C. En. Limited Reservoir et matiere de stockage de gaz d'hydrogene

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WO2001083090A1 (fr) * 2000-04-19 2001-11-08 Neubert, Susanne Membrane composite
WO2003052371A1 (fr) * 2001-12-18 2003-06-26 Inficon Gmbh Systeme de passage de gaz comprenant des surfaces de passage de gaz agissant de façon selective
US20030192779A1 (en) * 2002-04-15 2003-10-16 Yaw-Chung Cheng Device for charging and activating hydrogen storage canister
WO2005028945A2 (fr) * 2003-09-19 2005-03-31 Prototech As Stockage de fluides pressurises
WO2006046248A1 (fr) * 2004-10-27 2006-05-04 C. En. Limited Reservoir et matiere de stockage de gaz d'hydrogene

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US7813627B2 (en) 2006-09-29 2010-10-12 Praxair Technology, Inc. Low vapor pressure high purity gas delivery system
WO2008042710A3 (fr) * 2006-09-29 2008-07-03 Praxair Technology Inc Système de distribution de gaz très pur à faible tension de vapeur
WO2008042710A2 (fr) * 2006-09-29 2008-04-10 Praxair Technology, Inc. Système de distribution de gaz très pur à faible tension de vapeur
CN101542186B (zh) * 2006-09-29 2011-07-06 普莱克斯技术有限公司 低蒸汽压力的高纯度气体输送方法及输送系统
KR101185175B1 (ko) * 2007-11-08 2012-09-24 스턴 모쉬 마이크로실린더 배열에서 압축된 기체를 저장하고 유리하는장치 및 상기 마이크로실린더 배열들을 충전하는 시스템
EP2062850A2 (fr) 2007-11-08 2009-05-27 C. EN. Limited Appareil de stockage et libération de gaz hydrogène comprimé dans des réseaux microcylindriques et système de remplissage de réseaux microcylindriques
EP2062850A3 (fr) * 2007-11-08 2009-10-14 C. EN. Limited Appareil de stockage et libération de gaz hydrogène comprimé dans des réseaux microcylindriques et système de remplissage de réseaux microcylindriques
US7870878B2 (en) 2007-11-08 2011-01-18 C. En. Limited Apparatus for storage and liberation of compressed hydrogen gas in microcylindrical arrays and system for filling the microcylindrical arrays
WO2009090491A3 (fr) * 2007-11-30 2009-09-03 Honda Motor Co., Ltd. Systèmes de réchauffement pour dispositifs de stockage de gaz à haute pression
US8796600B2 (en) 2007-11-30 2014-08-05 Honda Motor Co., Ltd. Induction warming system for fiber composite gas storage cylinders
CN101504112B (zh) * 2008-02-07 2011-08-24 林德股份公司 加氢燃料的方法
DE102009016475A1 (de) 2008-04-01 2010-04-15 Deutsches Zentrum für Luft- und Raumfahrt e.V. Wasserstoffbereitstellungssystem und Verfahren zur Bereitstellung von Wasserstoff
DE102009016475B4 (de) * 2008-04-01 2012-02-02 Deutsches Zentrum für Luft- und Raumfahrt e.V. Wasserstoffbereitstellungssystem und Verfahren zur Bereitstellung von Wasserstoff
EP2163805A2 (fr) 2008-09-11 2010-03-17 C. En. Limited Appareil pour le stockage de gaz
US20140045089A1 (en) * 2008-12-23 2014-02-13 Encite Llc Gas Storage System
JP2012513572A (ja) * 2008-12-23 2012-06-14 エンサイト・エルエルシー ガス貯蔵システム
US9343757B2 (en) 2008-12-23 2016-05-17 Encite Llc Gas storage system
WO2011080746A1 (fr) * 2010-01-04 2011-07-07 C. En. Limited Appareil de stockage d'hydrogène gazeux comprimé dans des batteries de micro-cylindres
WO2013045043A1 (fr) * 2011-10-01 2013-04-04 Daimler Ag Dispositif destiné au stockage d'un combustible gazeux
DE102011087023A1 (de) 2011-11-24 2013-05-29 Helmholtz-Zentrum Berlin Für Materialien Und Energie Gmbh Verfahren und anordnung zur hochdruckspeicherung von wasserstoffgas
US9052063B2 (en) 2012-01-20 2015-06-09 L'Air Liquide Société Anonyme Pour L'Étude Device for storage of compressed gas, method of making the same, and method of using the same
WO2015019094A3 (fr) * 2013-08-08 2016-04-21 Intelligent Energy Limited Appareil et procédé de remplissage de gaz
US20160195219A1 (en) 2013-08-08 2016-07-07 Intelligent Energy Limited Gas filling apparatus and method
US10174882B2 (en) 2013-08-08 2019-01-08 Intelligent Energy Limited Gas filling apparatus and method
CN105715942A (zh) * 2014-12-05 2016-06-29 刘建华 内置cng气瓶玻璃钢储罐
WO2017037429A3 (fr) * 2015-08-28 2017-04-27 Intelligent Energy Limited Appareil de stockage de vase de dewar
US11137116B2 (en) 2015-08-28 2021-10-05 Intelligent Energy Limited Dewar vessel storage apparatus
CN113915525A (zh) * 2021-10-29 2022-01-11 江苏氢枫能源装备有限公司 一种固态储氢氢气吸附与释放装置
CN113915525B (zh) * 2021-10-29 2022-08-23 江苏氢枫能源装备有限公司 一种固态储氢氢气吸附与释放装置

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