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WO2025041021A1 - Source d'énergie renouvelable utilisant des processus et des systèmes de filtration entraînés par la pression - Google Patents

Source d'énergie renouvelable utilisant des processus et des systèmes de filtration entraînés par la pression Download PDF

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Publication number
WO2025041021A1
WO2025041021A1 PCT/IB2024/058000 IB2024058000W WO2025041021A1 WO 2025041021 A1 WO2025041021 A1 WO 2025041021A1 IB 2024058000 W IB2024058000 W IB 2024058000W WO 2025041021 A1 WO2025041021 A1 WO 2025041021A1
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Prior art keywords
membrane
water
feed
membrane element
group
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Pending
Application number
PCT/IB2024/058000
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English (en)
Inventor
Boris Liberman
Tomer EFRAT
Vitaly LEVITIN
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Ide Water Technologies Ltd
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Ide Water Technologies Ltd
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Publication date
Priority claimed from US18/497,768 external-priority patent/US20240075430A1/en
Application filed by Ide Water Technologies Ltd filed Critical Ide Water Technologies Ltd
Publication of WO2025041021A1 publication Critical patent/WO2025041021A1/fr
Priority to US19/098,901 priority Critical patent/US20250257482A1/en
Pending legal-status Critical Current
Anticipated expiration legal-status Critical

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D65/00—Accessories or auxiliary operations, in general, for separation processes or apparatus using semi-permeable membranes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D61/00—Processes of separation using semi-permeable membranes, e.g. dialysis, osmosis or ultrafiltration; Apparatus, accessories or auxiliary operations specially adapted therefor
    • B01D61/14—Ultrafiltration; Microfiltration
    • B01D61/20—Accessories; Auxiliary operations
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C25B1/01—Products
    • C25B1/02—Hydrogen or oxygen
    • C25B1/04—Hydrogen or oxygen by electrolysis of water
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B15/00—Operating or servicing cells
    • C25B15/08—Supplying or removing reactants or electrolytes; Regeneration of electrolytes
    • C25B15/085—Removing impurities
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
    • C25B9/23—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms comprising ion-exchange membranes in or on which electrode material is embedded
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/60—Constructional parts of cells
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2311/00—Details relating to membrane separation process operations and control
    • B01D2311/26—Further operations combined with membrane separation processes
    • B01D2311/2684—Electrochemical processes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2313/00—Details relating to membrane modules or apparatus
    • B01D2313/90—Additional auxiliary systems integrated with the module or apparatus
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/44—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis
    • C02F1/441—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis by reverse osmosis
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/44—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis
    • C02F1/442—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis by nanofiltration
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/44—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis
    • C02F1/444—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis by ultrafiltration or microfiltration
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/44—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis
    • C02F1/445—Treatment of water, waste water, or sewage by dialysis, osmosis or reverse osmosis by forward osmosis
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46133—Electrodes characterised by the material
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F1/00—Treatment of water, waste water, or sewage
    • C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
    • C02F1/461—Treatment of water, waste water, or sewage by electrochemical methods by electrolysis
    • C02F1/46104—Devices therefor; Their operating or servicing
    • C02F1/46109—Electrodes
    • C02F2001/46133—Electrodes characterised by the material
    • C02F2001/46138—Electrodes comprising a substrate and a coating
    • C02F2001/46142—Catalytic coating
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
    • C02F2103/08—Seawater, e.g. for desalination
    • C—CHEMISTRY; METALLURGY
    • C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
    • C02F2201/00—Apparatus for treatment of water, waste water or sewage
    • C02F2201/46—Apparatus for electrochemical processes
    • C02F2201/461—Electrolysis apparatus
    • C02F2201/46105—Details relating to the electrolytic devices
    • C02F2201/46115—Electrolytic cell with membranes or diaphragms

Definitions

  • the present invention relates generally to the production of a renewal energy source, in particular hydrogen, using pressure driven filtration processes and systems.
  • the present invention relates generally to the production of a desalinated, filtrated or other way treated water simultaneously with generation of renewal energy source, in particular hydrogen, using osmotic and/or gauge pressure driven filtration processes and systems
  • Water electrolysis technologies are known for producing hydrogen from water. Water is the reactant, which is dissociated to hydrogen and oxygen using a direct current.
  • a membrane element configured for osmotic and/or gauge pressure driven filtration of water and electrochemical splitting of at least a proportion of the water for the co-generation of hydrogen, the membrane element comprising at least one selectively permeable membrane configured to least partially purify feed water when a pressure difference is provided across the membrane, wherein the membrane element includes at least one anode electrode and at least one cathode electrode.
  • the selectively permeable membrane is any type of reverse osmosis (RO) or ultrafiltration (UF) type membrane that may be used for osmotic and/or gauge pressure driven filtration of water.
  • RO reverse osmosis
  • UF ultrafiltration
  • UF type of membrane includes those membranes used for ultrafiltration (UF), microfiltration (MF) and other purification from suspended solids processes. These types of membranes are selectively permeable with a maximum pore size of 0.1 microns.
  • the optional reject water outlet is for the reject flow which is the part of feed water which does not pass the membrane, being rejected as brine in selectively permeable membrane application. This reject flow may not exist in UF and MF applications.
  • the module may be provided with a hydrogen and/or oxygen outlet.
  • dissolved hydrogen and/or free gas hydrogen is provided in the reject flow or product water for later extraction therefrom, for example by degasification or gas separation membranes.
  • the membrane element according to the first aspect of the present invention and the module according to the second aspect of the invention may be incorporated into any pressure driven water filtration process or system to provide simultaneous cogeneration of at least partially purified water and hydrogen.
  • a third aspect of the present invention provides a process for pressure driven water filtration with co-generation of hydrogen, the process comprising: supplying feed water from a feed water inlet to a membrane element according to the first aspect of the present invention; applying a pressure differential across the RO and UF type selectively permeable membrane of the membrane element to draw feed water through the membrane to form a product water; applying a potential difference between the electrodes of the membrane element to cause electrochemical splitting of at least a portion of the feed and/or product water for formation of hydrogen and oxygen; and collecting the product water and optionally a reject flow, and hydrogen.
  • the hydrogen is dissolved in at least one of the product water or reject flow for subsequent extraction therefrom, for example by degasification or membrane gas separation.
  • the hydrogen could be in a free gas form.
  • a fourth aspect of the present invention provides a system for pressure-driven water filtration with the co-generation of hydrogen, the system comprising: a feed water inlet; at least one membrane element according to the first aspect of the present invention; at least one pump to apply a pressure to the feed water; a power source to provide a potential difference to the electrodes of the membrane element; a product outlet and optionally a reject water outlet; and a hydrogen outlet within the product and/or reject water.
  • the membrane element and module of the first and second aspects of the invention respectively may form part of a pressure retarded osmosis (PRO) system to provide electricity from the water with the co-generation of hydrogen.
  • PRO pressure retarded osmosis
  • the membrane element or module is incorporated into a reverse osmosis (RO) or Nano Filtration (NF) or other brand name system for the desalination of water and co-generation of hydrogen.
  • RO reverse osmosis
  • NF Nano Filtration
  • the element or module may be incorporated into any other water filtration system, such as ultrafiltration or microfiltration systems, to provide purified water and hydrogen generation, all of which are discussed further herein.
  • the main difference between RO; PRO; NF from UF and MF is that RO; PRO; NF implement salt rejection semipermeable membrane and have a reject flow.
  • the UF and MF membrane are not salt rejection semipermeable and do not have reject flow.
  • Electrodes within or on their membranes to allow water splitting in accordance with the invention.
  • RO Reverse Osmosis
  • NF Nano Filtration
  • PRO Pressure Retarded Osmosis
  • Water filtration processes and systems of the present invention include Ultra Filtration (UF) and Micro Filtration (MF) and other processes based on non- salt rejection semipermeable membranes in which water is moving through any membrane driven by gauge pressure for purpose of water treatment (purification from suspended solids), and hydrogen generation is a complementary co-generation activity.
  • UF Ultra Filtration
  • MF Micro Filtration
  • membrane implemented for UF, MF and other purification from suspended solids processes will be mentioned in one general name “UF type membrane”
  • inlets and outlets are dependent upon the type of desalination or water treatment process in relation to which the electrochemical splitting of water is incorporated.
  • the module has one inlet “Raw saline solution” and two outlets: “residual brine stream” (“reject flow” or “reject outlet”) and a “Permeate stream”. Hydrogen can go out from one or both of these outlets.
  • the module for a PRO process has two inlets and two outlets.
  • the process may also provide for pH correction to optimize the reaction taking place across the electrodes, for example to decrease the reversible potential of oxygen evolution reaction.
  • any type of RO and UF type membrane may be provided within the module for carrying out osmotic and/or gauge pressure-driven filtration of the feed water.
  • the membrane is adapted to include an anode and cathode and as an option an additional electrode to allow for electrochemical split of part of the penetrated water to generate hydrogen.
  • Suitable membranes incorporating these electrodes may be provided in a very wide range of configurations and are not limited to the specific permutations disclosed herein.
  • the membrane element or module may incorporate feed and/or permeate spacers.
  • the electrodes may be provided on or adjacent one or other of the feed and/or permeate spacers.
  • the salt rejection layer, support layer, feed or permeate spacers serve to act as mechanical supports for the electrodes.
  • the existing permeate and feed spacers of RO, PRO; NF, and FO modules, as well as semipermeable layers of RO; PRO; NF, and FO membranes can be used as is for separation of the anode and cathode electrodes incorporated into the membrane elements of the invention.
  • the cathode and anodes may be positioned on either one or both inside and/or outside of these hollow-fibres membranes.
  • the electrodes may be incorporated into the RO type membrane in many different configurations.
  • the at least two electrodes may be provided between the salt rejection and the support layers.
  • at least one electrode may be positioned between the salt rejection layer and the support layer and at least one electrode may be provided on an external surface of the salt rejection layer.
  • the at least two electrodes may both be provided on an external surface of the salt rejection layer.
  • the electrodes may be located on permeate and/or feed spacers, more preferably the electrodes are positioned on either side of the permeate or feed spacer.
  • both electrodes may be located on one side of permeate and/or feed spacers.
  • one electrode may be located on one side of permeate and/or feed spacers and the other electrodes may be located on opposite site of permeate and/or feed spacers.
  • the electrode anode and/or cathode
  • the feed spacer is mechanically coupled to the permeate tube.
  • the anode may be coupled to the feed spacer and the cathode may be coupled to the permeate spacer.
  • the cathode may be coupled to the feed spacer and the anode may be coupled to the permeate spacer.
  • the polarity of the spacers may be alterable so as to control which electrode is utilized as the cathode and which as the anode.
  • the electrode may comprise the feed and/or permeate spacer.
  • the spacer is at least partially coated with an electrically conductive layer and/or a catalytic layer, thereby making the electrode electrically conductive and electrocatalytically active as anodes (for O2 evolution) or electrocatalytically active as cathodes (for H 2 evolution) or both.
  • the spacers may be at least partially coated with at least one catalyst, for example being selected from Pt, Ir and any combination thereof.
  • the conductivity of the spacers may be obtained via, for example, coating of the polymer spacer with a nickel or copper metal and then displacing these metals with a Pt- or Ir-group catalyst, for example by redox displacement or other techniques.
  • the electrodes may be provided in the form of a grid or parallel spaced apart strips.
  • the electrodes may be provided in the form of a full or partial coating of the permeate and/or feed spacer.
  • the salt rejection layer or spacers may be formed of a material that may allow them to serve as one of the electrodes, i.e., of a material having sufficient conductivity (such as e.g., graphite, composite of polymer and conductive particles, or metals). More preferably still, the at least one electrode may be formed from graphene. In one embodiment, the electrode (anode and/or cathode) is graphene or carbon fiber/carbon cloth.
  • the carbons are substrates for coating with mixed metal oxides (MMO) selected from platinum (Pt), iridium (Ir), Pt-lr, ruthenium (Ru) metals, Cobalt, Nickel, and any combinations thereof.
  • MMO mixed metal oxides
  • the MMO/C electrodes may be prepared by a two-step process comprising forming a sacrificial copper or nickel layer on the carbon via electroless or electrodeposition and displacing the sacrificial metal by Pt, Ir, Ru or Pt-lr.
  • the salt rejection layer may be formed from graphene and comprise one of the electrodes.
  • the support layer is preferably comprised of a porous material, preferably being a ceramic material.
  • the electrode (anode and/or cathode) may be a titanium material to enhance durability.
  • the electrode may be provided in any configuration but is preferably selected from the group consisting of a mesh, plate, foil, cloth formed of fiber and a sintered body, more preferably being made of titanium.
  • the semi-permeable membrane may further comprise a reference electrode.
  • at least one dielectric material may be provided between the at least two electrodes.
  • the feed and/or permeate spacers may act as a dielectric material for the electrodes printed, coated or located on each side of the spacer(s).
  • At least one catalyst may be provided on at least one or both of the electrodes to enhance the desired reaction, for example to facilitate oxygen and hydrogen generation and hamper chlorine evolution.
  • the electrode may be at least partially coated with at least one catalyst.
  • the catalyst is selected from at least one of the group consisting of iridium oxide, ruthenium oxide, tantalum oxide, titanium oxide, platinum, and platinum oxide, Cobalt, Cobalt oxide, Nickel, Nickel oxide and any combination thereof.
  • the process and system according to the third and fourth aspects of the invention may be applied to many different types of pressure driven water filtration processes and systems.
  • the process and system comprise a reverse osmosis (RO) process and system for splitting water to hydrogen and oxygen in an osmosis separation module comprising at least one, preferably multiple membrane elements, said membrane having a feed side and permeate side with the at least two electrodes positioned on the RO type membrane, and/or support layer, and/or feed and/or permeate spacers of the membrane element.
  • RO reverse osmosis
  • Raw saline solution is delivered to the module and a part of the raw saline solution exits the module as a residual brine stream, part of the raw saline solution penetrating the membrane in a normal reverse osmosis process to produce desalinated water by a net driving force of the balance of the gauge and osmotic pressures and exiting from a permeate side of the membrane element as a permeate stream.
  • the process includes applying continuously, or for a predetermined period, electrical current to membrane electrodes, which causes part of the raw saline solution and/or permeate stream to be split into hydrogen and oxygen gases for evacuation from the osmosis separation module together with the residual brine stream and/or permeate stream.
  • the RO module combines desalination of raw saline solution for commercial use with the simultaneous splitting of water into hydrogen and oxygen.
  • less then 5% of raw saline solution is used for hydrogen generation, more preferably less than 1%.
  • the process and system may be applied to a water purification process conducted on non- salt rejection semipermeable membrane such as Ultra Filtration and Microfiltration membrane in UF or MF process.
  • non- salt rejection semipermeable membrane such as Ultra Filtration and Microfiltration membrane in UF or MF process.
  • less than 1% of filtered water is used for hydrogen generation, preferably less then 0.1% of filtered water.
  • Such a process and system for providing filtration of water and cogeneration of hydrogen may include a suspended solids fouling filtration module, said membrane element having a feed side and filtered side with at least two electrodes positioned on the membrane, and/or the support layer, and/or the feed and/or filtered water spacers, wherein a raw saline solution enters the feed stream side of the module, and at least partially penetrates the membrane in a normal filtration process by a driving force of the gauge pressures and exits from the filtered side as a filtered stream, said method for splitting water to hydrogen and oxygen comprising: applying continuously, or for a predetermined period, electrical current to the electrodes, which cause part of the permeate stream to be split into hydrogen and oxygen gas for evacuation from the filtration module together with the filtered water stream.
  • an osmotic process and system for the splitting of water to hydrogen and oxygen comprising delivering first and second solutions of different osmotic and gauge pressures to opposing sides of a RO type semi-permeable membrane to create a low salinity solution across the membrane; the semi-permeable membrane including at least two electrodes; applying a current across the electrodes of the RO type semi-permeable membrane to split the low salinity solution into hydrogen and oxygen; and collecting the hydrogen and oxygen (both either dissolved and/or free gas).
  • the first solution is known as the draw solution and the second solution is known as the feed solution.
  • the feed solution may comprise sea water, brackish water, wastewater or fresh water, such as river or ground water.
  • the osmotic process may comprise pressure retarded osmosis or forward osmosis wherein the RO type semi-permeable membrane has a first side and a second side opposite the first side; a first saline solution comprising the draw solution having an osmotic pressure POr and a gauge pressure PGr for entering the first side of the membrane; a second saline solution comprising a feed solution having an osmotic pressure POp and a gauge pressure PGp for entering the second side of the membrane; at least part of the feed solution from the second side of the membrane penetrating to the first side according to a net driving pressure defined by the balance of pressures PGr, POr, POp and PGp; wherein the draw solution and the penetrated part of the feed solution exit as a residual brine stream from the first side of the membrane via a residual brine outlet; a remainder of the feed solution at least periodically exits as a residual fluid stream from the second side of the membrane via an outlet and wherein at least part of
  • the processes and systems according to the third and fourth aspects of the invention may, and preferably do, incorporate conventional steps and components for carrying out these processes and systems that are used in the prior art processes and systems.
  • the generated hydrogen may be stored in holding tanks for later use or fed into a network grid for use.
  • Figure 1 A is a schematic diagram illustrating the principle of alkaline water electrolysis according to the prior art
  • FIG. 1 B is a schematic diagram illustrating the principle of proton exchange membrane (PEM) water electrolysis according to the prior art
  • Figure 2A is a schematic top view of a section through FO or PRO semi-permeable membrane incorporating electrodes according to an embodiment of the present invention
  • Figure 2B is a three-dimensional view of the semi-permeable membrane shown in Figure 2A, with the salt rejection layer 4 and feed 7 removed;
  • Figure 3 is a three-dimensional view of a semi-permeable membrane incorporating a pair of electrodes according to an alternative embodiment of the present invention
  • Figure 4 is a three-dimensional view of a semi-permeable membrane incorporating a pair of electrodes according to yet another embodiment of the present invention.
  • Figure 5 is a three-dimensional view of a semi-permeable membrane incorporating a pair of electrodes according to still yet another embodiment of the present invention.
  • Figure 6A is a fragmented three-dimensional view of a semi-permeable membrane having permeate and feed spacers and incorporating electrodes according to yet a further embodiment of the present invention
  • Figure 6B illustrates two membranes according to Figure 6A arranged in mirror symmetry
  • Figure 7 is a schematic diagram of a seawater desalination plant and process scheme in which one or more semi-permeable membranes according to the invention may be incorporated;
  • Figure 8 is a graph of reversible potentials for chlorine evolution, oxygen evolution and hydrogen evolution reactions as a function of pH.
  • Figure 9 is schematic diagram illustrating an embodiment of a system of the present invention for hydrogen generation and storage
  • Figure 10 is a schematic diagram of a permeate tube with a pair of spacers and electrodes coupled thereto according to an embodiment of the invention.
  • Figure 11 is a schematic diagram of a permeate tube with multiple spacers and electrodes coupled thereto according to another embodiment of the invention.
  • Figure 12 is a schematic diagram of a Titanium foil cladding 300 to permeate and/or feed spacers with and without additional electricity conductors between titanium foil and plastic spacer.
  • Figures 13-14 are schematic diagrams providing different examples of corrugation (or embossing) patterns.
  • Figure 15 illustrates an embodiment where the electrode (e.g., the Titanium foil) substitutes at least one selected from a group consisting of permeate spacer, feed spacer and any combination thereof.
  • the electrode e.g., the Titanium foil
  • FIGs 16-22 are schematic diagrams of coupling between the electrode, which could serve as the spacers (permeate and/or feed spacers) and the permeate tube.
  • Figures 23-25 are schematic diagrams of embodiments utilizing bi-polar electrodes.
  • Figures 26-28 are schematic diagrams of embodiments utilizing another embodiment where at least a portion of the spacers (feed spacers and/or permeate spacers) are joint together.
  • the present invention relates generally to the novel generation of hydrogen from water produced during water desalination or water treatment processes that use RO or UF- type membranes, wherein feed water is pressure driven (for example by osmotic and gauge pressures) against the membrane to allow certain components to pass through the membrane while other components are rejected, with a proportion of the water being split electrochemically to produce hydrogen.
  • the process utilises feed water penetrated via RO type semipermeable membrane in to draw solution during pressure retarded osmosis process PRO, or forward osmosis FO.
  • the very low salinity water passes via the RO type semi-permeable membrane from feed stream to draw solution stream.
  • a small portion of this very low salinity water is subjected to electrolysis thereby splitting the water to produce hydrogen.
  • This is achieved by the incorporation of one or electrodes into the RO type semi-permeable membranes conventionally used in these pressure- driven energy generation processes to provide modified membranes that allow simultaneous splitting of the water via electrolysis in addition to the standard PRO conventionally carried out process using these types of membrane.
  • Pressure retarded osmosis is an osmotically driven membrane process that uses energy harnessed from the mixing between high and low salinity streams to produce mechanical energy (utilization of Gibb’s free energy of mixing).
  • Water permeates through RO type semi-permeable membranes from a low concentration feed stream into a high concentration, partially pressurized, brine stream (“draw solution”).
  • the hydraulic pressure is less than its osmotic pressure resulting in a net osmotic driving force for transport of water (permeate stream) from the feed stream to the brine stream.
  • the permeate stream becomes pressurised and dilutes the brine stream and the energy in the pressurised permeate stream can be converted into mechanical or electrical energy via a turbine generator.
  • Forward osmosis is an alternative osmotically driven membrane process that uses the RO type membrane to treat two liquid feed streams.
  • One side of the membrane is a feed solution (FS) with a low osmotic pressure and the other side of the membrane is the draw solution (DS) with a higher osmotic pressure.
  • FS feed solution
  • DS draw solution
  • the difference in osmotic pressure causes water to pass through the membrane from the FS side to the DS side, simultaneously diluting the DS and concentrating the FS.
  • the RO type membranes consist of an active layer (or salt rejection layer) and a porous support layer, with the FS side generally facing the active layer.
  • a RO type semipermeable membrane is basically a very thin layer of polymeric material that acts as a barrier layer and separates dissolved ions or molecules from water when the applied pressure is greater than osmotic pressure.
  • the present invention utilizes a permeate stream produced during PRO or FO. This stream cannot be directly measured because it cannot be extracted from the membrane and is extremely thin. However, the inventors have recognized for the first time that this stream may be used for hydrogen production due to its extremely low salinity.
  • the present innovation positions electrodes in this extremely thin low salinity stream for the purpose of water split for hydrogen and oxygen production.
  • the present invention provides novel permeable membranes for enabling water split and furthermore, provides a novel method and system for generating hydrogen and oxygen from water.
  • the invention may also be incorporated into RO and NF processes wherein a small portion of the raw salinity feed water and/or permeate water is subjected to electrolysis thereby splitting the water to produce hydrogen.
  • This is again achieved by the incorporation of one or electrodes into the RO type semi-permeable membranes conventionally used in these pressure-driven water desalination processes to provide modified membranes that allow simultaneous splitting of the water via electrolysis in addition to the standard water desalination conventionally carried out using RO type of membrane.
  • the invention may be incorporated into UF and MF processes wherein a small portion of the feed water and/or filtrated water is subjected to electrolysis thereby splitting the water to produce hydrogen.
  • This is again achieved by the incorporation of one or electrodes into the UF type of membranes conventionally used in these pressure-driven water treatment processes to provide modified membranes that allow simultaneous splitting of the water via electrolysis in addition to the standard water treatment conventionally carried out using UF types of membrane.
  • RO; NF; PRO; UF; MF processes that be modified according to the invention to provide hydrogen generation.
  • the invention provides for simultaneous water desalination (RO, NF) or water treatment (UF, MF, FO) or osmotic power generation (PRO) and electrochemical production of hydrogen gas for conversion and storage of electrical energy (hydrogen economy).
  • Electrochemical and membrane reactors have at least two common components: spacers and membranes. Moreover, modern water electrolysis systems utilize ultra-pure water.
  • Electrolysis of deionized water directly in a desalination or filtration module using same membranes, spacers, control and automation units, hydraulic system, and other equipment and materials will reduce drastically operational and capital costs of water electrolysis and will provide an added value to the desalination or water treatment plants.
  • All WE techniques are based on oxidation and reduction of water molecules or H+ and OH- ions into oxygen and hydrogen gases on anodes and cathodes. These processes consume electrical energy and heat with the reaction occurring at the anodes and cathodes being dependent upon the pH in the electrolyzed solution, as set out below:
  • the oxidation and reduction processes proceed on the anodes and cathodes, respectively.
  • the anodes are more positive than the cathodes.
  • the electrons flow from anodes to cathodes (i.e., in the direction opposite to a flow of electric current) through an external wire (or other, normally metallic conductors) connected to a direct current (DC) supply.
  • the electrical circuit of the electrochemical cell requires movement of electrical charges (i.e., ions) in the electrolyzed solution. In other words, an electrolyte must be present in water to sustain the WE process.
  • Two major types of electrolytes are used in low temperature (i.e., T ⁇ 100°C) water electrolysis processes: (1 ) salts, acids, and bases; and (2) solid electrolytes.
  • solid electrolyte refers to an ion-exchange membrane which is located between anode and cathode in an electrochemical cell. Normally polymeric cation-exchange membranes (e.g., National, the sulphonated tetrafluoroethylene-based fluoropolymer-copolymer) are used in this type of WE devices.
  • PEM proto exchange membrane
  • the membrane in its original form contains fixed negatively charged sulfonic groups and exchangeable H+ ions.
  • Anodic production of oxygen via reaction Eq. (3) results in generation of H+ ions.
  • These ions flow through the membrane (ionic current in a “solid” electrolyte) and get consumed within the hydrogen evolution reaction that proceeds on a cathode via reaction Eq. (4). This way the overall concentration of H+ ions in the membrane remains constant.
  • the PEM electrolyzes requires ultra-pure deionized water (less than 0.5 ppm of total dissolved solids to prevent deterioration of membranes) and expensive noble metal catalysts (e.g., lrC>2 for anodes and Pt for cathodes).
  • These conventional water electrolysis processes require ionic carriers that can be (1 ) originally present in the electrolyzed water (e.g., seawater), (2) added into deionized water (e.g., alkaline water electrolysis), or (3) provided with the ion-exchange membranes. Electrolysis of pure water is not generally carried out.
  • Seawater is potentially an endless source of water for electrochemical generation of hydrogen.
  • seawater contains significant amounts of magnesium and calcium ions that precipitate in alkaline solutions and/or on a cathode due to the high local pH that exists in the near cathode area because of hydrogen evolution reaction.
  • seawater contains high concentrations of chloride ions that can be oxidized on an anode to produce chlorine gas. This is then hydrolyzed into hypochlorous acid (HOCI) which exists in equilibrium with hypochlorite ions (OCI ).
  • HOCI hypochlorous acid
  • OCI hypochlorite ions
  • CI2 is the primary anodic product if direct seawater electrolysis process is performed using typical water electrolysis anodes (e.g., graphite, Pt, mixed metal oxides, lrC>2, etc.). Production of chlorine in seawater electrolysis aimed at mass production of H 2 must be prevented.
  • the present invention reduces or eliminates all these problems by the incorporation of electrodes into the conventional pressure-driven membranes utilized in desalination or water treatment processes. This represents a significant step forward in the generation of hydrogen from accessible water sources.
  • the processes and systems of the present invention which perform simultaneously pressure-driven membrane filtration of water with electrochemical splitting of water to produce hydrogen are very different to the prior art large scale electrochemical splitting of water.
  • the integration of electrochemical process into the water desalination or filtration modules according to the present invention is not expected to result in a larger footprint of desalination or water treatment facilities already in existence.
  • operational costs are expected to be even lower than the well-established water electrolysis technologies.
  • desalinated water includes Ca, Mg, Na, CO3, SO4, HCO3, Cl and other ions in an amount 10 to 300ppm.
  • concentration of dissolved solids in permeate water stream is increasing. If all permeate is used for split, two problems will arise; (i) scaling formation CaCOs, CaSC etc and (ii) increased conductivity of permeate which will increase power consumption for hydrogen generation.
  • the combination of two processes (desalination and split), (energy generation and split) or (water filtration and split) in one membrane element solves this contradiction.
  • the invention is cost efficient because common water pumping and water filtration equipment is used for the two combined processes.
  • Any pressure-driven membrane that provides for desalination or filtration of water may be adapted to simultaneously produce hydrogen according to the present invention, such as RO, NF, PRO, FO, UF and MF membranes.
  • RO-type or UF-type membranes are referred to as RO-type or UF-type membranes and generally these consist of semi-permeable membranes with a maximum pore size of 0.1 microns.
  • the type of membrane will have a particular pore size, for example MF membranes generally have a maximum pore size of about 0.1 microns; UF membranes generally have a pore size of 0.01 to 0.1 microns; NF membranes generally have a maximum pore size of 0.01 microns and RO membranes generally have a pore size of 0.0001 microns.
  • FIGS 2A and 2B of the accompanying drawings illustrate one embodiment of a novel semi-permeable membrane 3 according to the present invention which may be incorporated into a PRO or FO module to carry out the process as described above.
  • the membrane is provided with electrodes 9, 10 which enable it to be used for hydrogen generation in addition to its conventional use.
  • a feed stream (saline solution, FS) 7 is delivered to a feed side 2 of the semipermeable membrane 3.
  • the membrane 3 consists of a salt rejection layer 4 and support layer 5 with a series of parallel electrodes 9, 10 positioned between the salt rejection layer 4 and the support layer 5.
  • part of the feed stream 7 (saline solution) moves from the feed side 2 of semipermeable membrane through the salt rejection layer 4 (omitted from Figure 1 B for sake of simplicity) and support layer 5 to the opposite side 1 (draw side) as permeate 8.
  • This permeate stream 8 has a very low salinity (around 2%) and thus has an osmotic pressure lower than the feed stream 7 (POf) and lower than the draw solution stream 6 (POr).
  • FIGS 3, 4 and 5 of the accompanying drawings illustrate alternative embodiments of semi-permeable membranes 3 according to the present invention, the membranes 3 being provided with electrodes 9, 10 in different positions within the membrane.
  • Identical features already discussed in relation to Figures 2A and 2B are given the same reference numerals.
  • Figure 3 shows the membrane 3 with both electrodes 9, 10 (anode and cathode) positioned externally on the surface of the salt rejection layer 4.
  • Figure 4 shows membrane 3 with both electrodes 9, 10 positioned between the support layer 5 and the salt rejection layer 4.
  • one electrode 10 is positioned between the support layer 5 and the salt rejection layer 4 with the other electrode 9 positioned on an external surface of the salt rejection layer 4.
  • the semi-permeable membrane may comprise a module having a permeate tube and flat membrane sheets wound around the tube to provide a membrane element and incorporating permeate and/or feed spacers (supporting layers between the membrane sheets).
  • These types of membrane elements or modules may also be adapted to incorporate electrodes in accordance with the present invention.
  • Figure 6A shows a fragment of such a membrane 3 arrangement. It is single fragment of RO membrane with raw feed flow 42 and permeate flow 43. Support layer 5 and salt rejection layer 4 forms entire membrane 3.
  • a permeate spacer 41 is provided on the support layer side 5 of membrane 3 and a feed spacer 40 is provided on the salt rejection side 4 of membrane 3. This is a typical arrangement presented in Fig-6A. However, it is to be appreciated that other arrangements may be provided, such as positioning salt rejection layer 4 facing permeate spacer 41. Electrodes 9 and 10 are positioned on opposite sides of permeate spacer 41 . In another embodiment, electrodes may be positioned on the same side (not shown). In other embodiments, three and more electrodes may be positioned on the same side or on both sides of permeate spacer 41 (again not shown).
  • one, two, three and more electrodes may be positioned on the same side or on both sides of the permeate spacer 41 and/or on feed spacer 40 (not shown).
  • This arrangement of electrodes positioned on feed spacer 40 and/or permeate spacer 41 may be combined with electrodes positioned on salt rejection layer 4 and support layers 5 of membrane 3 as described above.
  • the position of the salt rejection layer in some membranes may be orientated to permeate channel instead of feed channel (again this is not shown in the accompanying figures).
  • the electrodes 9, 10 may be incorporated into multiple types of filtration membranes and are not limited to those shown and described herein. This includes membranes that may consist entirely of a salt rejection layer 4 and do not have support layer 5 and/or feed or permeate spacers.
  • Figure 6B shows a fragment of two membranes 3 arranged in mirror symmetry in RO module with arrows for the raw feed flow 42 and arrows for the permeate flow 43 passing between membranes 3.
  • Permeate flow generated on the membrane 3 is shown as arrow 44, which joins permeate flow 43 coming from other membranes positioned in the module.
  • any type, number and arrangement of electrodes may be provided within the membrane to allow water splitting to be carried out.
  • Two or multiple electrodes may be installed between salt rejection and support layers, the electrodes can be installed in the support layer only, in rejection layer only or the electrodes can be installed in both layers.
  • the electrodes must have the necessary conductivity and one of the electrodes may comprise the active or salt rejection layer 4.
  • a preferred embodiment of the semi- permeable membrane has a salt rejection layer that also forms one of the electrodes.
  • One preferred material for the electrode, which may also comprise the active or salt rejection layer 4 is graphene. However, another suitable material is titanium.
  • the substrate for the electrode may, for example, comprise a mesh, plate, foil, cloth formed of fiber or a sintered body. Dielectric layers may also be incorporated into the membranes between the electrodes. The layers may be interconnected and may be produced by techniques such as casting or printing, gluing or growing.
  • the electrode may also be at least partially coated with at least one catalyst, such as one selected from the group consisting of iridium oxide, ruthenium oxide, tantalum oxide, titanium oxide, platinum, and platinum oxide, Cobalt, Cobalt oxide, Nickel, Nickel oxide and any combination thereof.
  • the carbon substrate is preferably coated with mixed metal oxides (MMO) selected from Pt, Ir, Pt-lr and Ru metals and any combination thereof.
  • the carbons are substrates for coating with mixed metal oxides (MMO) selected from platinum (Pt), iridium (Ir), Pt-lr, ruthenium (Ru) Cobalt, Nickel metals and any combinations thereof.
  • MMO mixed metal oxides
  • the MMO/C electrodes may be prepared by a two-step process comprising forming a sacrificial copper or nickel layer on the carbon via electroless or electrodeposition and displacing the sacrificial metal by Pt, Ir, Ru or Pt-lr.
  • the present application is equally suitable for two, three or more electrode systems, such as cathode, anode and reference electrodes, or other. Additional non salt rejection layers (membranes) can be installed near to the electrodes.
  • feed spacers are used in spiral wound reverse osmosis membrane modules to keep the membrane sheets apart as well as to enhance mixing. They are beneficial to membrane performance but at the expense of additional pressure loss.
  • the feed spacers are a netting material placed between the flat sheets of a reverse osmosis membrane to promote turbulence in the feed / concentrate stream.
  • feed spacers are made of plastic polypropylene.
  • a permeate or channel spacer is also known as a "permeate water carrier", or “mesh spacer".
  • the permeate spacer is placed between two layers of the flat sheet membrane. This spacer is used to prevent the RO membrane from closing-off on itself under the high pressure of operation. Permeate water will flow in a spiral path across the product channel spacer into the product collection tube.
  • the permeate spacer is inside the envelope and creates a flow pass for permeate water. Additionally, it supports the membrane sheets mechanically against (high) feed pressure and therefore it is made of woven spacers with low permeability to have the required stiffness.
  • permeate or channel spacers are made of woven thin plastic (e.g., a knit fabric called Tricot).
  • the electrode may also comprise the feed or permeate spacer as discussed above, for example wherein the spacer is at least partially coated with an electrically conductive layer to make the spacer electrically conductive and/or a catalytic layer to make them electrocatalytically active as anodes (O2 evolution) or cathodes (H 2 evolution) or both.
  • the catalyst may be for example Pt, Ir, Ni, Cu metals or any combination thereof.
  • the electrode may be coupled to the permeate or feed spacer, which is in mechanical co-operation with the permeate tube.
  • An example of such an embodiment is shown in Figure 10 of the accompanying drawings wherein two electrodes 402 are coupled to spacers attached at one end to a permeate tube 400. Any number of electrodes and spacers may be provided, as shown in Figure 1 1 which has 20 electrodes 402, coupled to spacers, which are coupled at one end to the permeate tube 400.
  • the electrode is essentially the Titanium foil cladding.
  • Titanium foil acts essentially as the permeate and/or feed spacers.
  • the Titanium foil is by itself coupled to the permeate tube (further disclosure will be provided hereinabelow).
  • Titanium foil 300 is cladded to the permeate spacer 41 .
  • such cladding could be performed to the feed spacer 40 as well.
  • the cladding is performed on one side of the permeate and/or feed spacers. According to another embodiment, such cladding is performed on both sides of the permeate and/or feed spacers.
  • the cladding my be done by application of vacuum.
  • the foil is positioned and on the other side vacuum is applied.
  • suction will adhere the Titanium foil 300 to the permeate and/or feed spacers.
  • the thickness of such Titanium foil 300 can be varied and depending of the electrical conductivity needed.
  • electrical wires can be added to enable the electrical current transfer.
  • electrical wires 301 are also added to the permeate spacer 41.
  • the Titanium foil is incorporated into the membrane module (assembly) and acts as the electrode (anode and/or cathode).
  • the electrode anode and/or cathode.
  • the thickness of the electrode ranges between 1 micron (0.001 mm) to as thick as 3 mm.
  • the electrode e.g., the Titanium foil
  • the electrode is at least partially corrugated (embossed) in a predetermined pattern. It is within the scope of the present invention where the term corrugation refers to the act of shaping a surface of the corrugated element; in this case, the Titanium foil.
  • Corrugations are measured and categorized by the depth and spacing.
  • the size of the corrugations determines the culvert roughness used, according to some embodiments, corrugations are measured from crest to crest (width or pitch) and valley to crest (depth).
  • Figs. 13-14 providing examples of different corrugation patterns that can be used. However, it is within the scope of the present invention to provide any corrugating pattern (embossing pattern).
  • the electrode e.g., the Titanium foil
  • the electrode is only partially corrugated and not corrugated along its entire cross section/length.
  • the electrode e.g., the Titanium foil
  • the electrode is cladded onto at least one selected from a group consisting of permeate spacer, feed spacer and any combination thereof.
  • the electrode functions essentially as at least one selected from a group consisting of permeate spacer, feed spacer and any combination thereof.
  • the membrane element which comprises the at least 2 membranes enveloping at least one permeate spacer 208. And in between at least 2 membranes elements, at least one feed spacer 206 is provided.
  • the electrode e.g., the Titanium foil
  • the electrode substitutes at least one selected from a group consisting of permeate spacer, feed spacer and any combination thereof.
  • Figure 15 illustrating such an embodiment.
  • the electrode e.g., titanium replaces the feed spacer 206 (and thus, acting as the anode).
  • the titanium electrode can also replace the permeate spacer 208 (and thus, acting as the cathode for the generation of hydrogen).
  • At least one catalyst may be provided on at least one or both of the electrodes (cathode and/or anode) to enhance the desired reaction, for example to facilitate oxygen and hydrogen generation and hamper chlorine evolution.
  • the electrodes may be at least partially coated with at least one catalyst.
  • the catalyst is selected from at least one of the group consisting of iridium oxide, ruthenium oxide, tantalum oxide, titanium oxide, platinum, and platinum oxide, Cobalt, Cobalt oxide, Nickel, Nickel oxide and any combination thereof.
  • the Titanium electrode (anode and/or cathode) can be both at least partially corrugated and at least partially coated with the catalyst.
  • each of the electrodes/anodes/feed spacer or electrodes/cathodes/permeate spacer is corrugated substantially the same.
  • each of the electrodes/anodes/feed spacer or electrodes/cathodes/permeate spacer is corrugated in a substantially different manner.
  • Figs. 15a-15b illustrate waves-like corrugation pattern of the spacers (Fig. 15a. illustrates the corrugation pattern of the permeate spacer; and Fig. 15b illustrates corrugation pattern of the feed spacer).
  • the electrodes/anodes/feed spacer is waves-like corrugated in one direction
  • the electrodes/anodes/feed spacer is waves-like corrugated in one direction which is substantially different than the electrodes/anodes/feed spacer’s corrugation.
  • the corrugation of the electrodes/anodes/feed spacer is in 90 degrees relative to the corrugation of the electrodes/anodes/permeate spacer.
  • the waves-like corrugation of the permeate spacer is directed towards the permeate tube 1602 in order to facilitate the flow of the permeate towards the permeate tube 1602.
  • the waves-like corrugation pattern of the feed spacer is rotated at 90 degrees relative to the waves-like corrugation pattern of the permeate spacer.
  • the Titanium electrode (anode and/or cathode), which could serve as the spacers (permeate and/or feed spacers) is in physical connection with the permeate tube.
  • the coupling/anchoring means could be any mechanical coupling means (e.g., rivets, screws, etc.) 1601 , connecting the Titanium electrode 1600 to the permeate tube 1602.
  • an additional strips/flats bars 1604 could be provided to better secure the Titanium electrode 1600 to the permeate tube 1602.
  • openings 1700 located on the permeate tube 1602 (for the collection of the permeate water/the product).
  • the openings 1700 are disposed on the permeate tube and according to another embodiment, the openings 1700 could also be positioned on the coupling/anchoring means 1601 (e.g., rivets with internal openings, as illustrated in figure 17a).
  • the coupling/anchoring means 1601 e.g., rivets with internal openings, as illustrated in figure 17a.
  • FIG 17c illustrating a cross section area of the permeate tube 1602.
  • the assembly of the titanium electrode 1600 functioning as permeate spacer 208 and/or as feed spacer 206 is illustrated.
  • the membrane 1600/204 disposed between permeate spacer 1600/208 and feed spacer.
  • the coupling means e.g., rivets, screws, etc.
  • openings 1701 may be provided. Such openings 1701 are opening integrated in the coupling means 1601.
  • the electrode 1600 functioning as permeate spacer 208 and/or as feed spacer 206 is simply welded to the permeate tube 1602.
  • the titanium electrode 1600 functioning as permeate spacer 208 is welded to the permeate tube 1602.
  • the permeate tube 1602 comprises at least one groove, 1603 into which the electrode will be disposed.
  • Figure 18 illustrates the permeate tube 1602 with the grooves 1603
  • Figure 19 illustrates the assembly of permeate tube 1602 with the Titanium electrodes (permeate spacer or feed spacer) and the membranes.
  • the permeate spacer-Titanium electrode 208 is disposed within grooves 1603 (not shown) and at least one anchoring element 1604.
  • the anchoring element 1604 is adapted to be at least partially disposed within groove 1603, thereby securing the permeate spacer-Titanium electrode 208 within groove 1603 of the permeate spacer 1602.
  • openings 1700 located on the permeate tube 1602 (for the collection of the permeate water/the product).
  • the anchoring element 1604 is rubber-based anchoring.
  • the anchoring element is characterized by a cross- sectional shape selected from circular, elliptical, oval, rectangular, triangular, any combination thereof; or any other shape.
  • the RO membrane, 204 and the feed spacer, 206 are also illustrated in the figure.
  • the feed spacer 206 could also be Titanium electrode.
  • Figures 20-22 illustrating another embodiment of the present invention. According to which the permeate tube 1602 comprises a plurality of rod-like elements 1602a secured together.
  • the permeate spacer 208 comprises at least one bulging/protrusion element 2081 located on one peripheral end thereof.
  • the bulging/protrusion element 2081 is disposed in between each two rod-like elements 1602a.
  • the coupling between all rod-like elements 1602a to form the permeate tube 1206 essentially provide the coupling of the permeate spacer 208 to the permeate tube 1206.
  • the electrode e.g., Titanium electrode
  • the spacers feed or permeate
  • replacing the same and essentially functioning in the same manner.
  • Titanium electrode could be in the form of mesh, foil, plate, cloth, fiber, sintered body and any combination thereof.
  • the Titanium electrodes could be at least partially coated with at least one catalyst.
  • the catalyst is selected from a group consisting of iridium oxide, ruthenium oxide, tantalum oxide, titanium oxide, platinum, and platinum oxide, Cobalt, Cobalt oxide, Nickel, Nickel oxide and any combination thereof.
  • At least one of the Titanium electrodes could be at least partially corrugated (as illustrated in Figures 13-14).
  • the electrode can be incorporated within the element to allow electrochemical splitting of raw saline solution and/or permeate to create a smaller output of hydrogen generation together with a main output of residual brine stream and/or permeate product water.
  • bi-polar electrodes are utilized.
  • a bipolar electrode is defined as a floating conductor that can induce electrochemical reactions at its extremities when a sufficient voltage bias is applied to the opposing driving electrodes.
  • the two outermost anode and cathode (monopolar) are connected to an external electric power supply and internal electrodes are bipolar.
  • the internal bipolar electrodes possess antithetical (opposed) charges on its two sides.
  • Bipolar electrochemistry (and use of bipolar electrode) is a phenomenon in electrochemistry based on the polarization of conducting objects in electric fields. Indeed, this polarization generates a potential difference between the two extremities of the substrate that is equal to the electric field value multiplied by the size of the object.
  • the bi-polar electrode(s) is(are) floating and is(are) not connected to DC power supply. Only the two terminal electrodes (monopolar) are connected to power supply. Therefore, the system can be free of ohmic losses in the electrodes.
  • At least one membrane 204, at least one cathode 208, at least one anode, 206 and at least one floating electrode 230 is used.
  • At least one floating electrode 230 is in mechanical communication with at least one membrane 204.
  • Figs. 24-25 illustrating such embodiment.
  • Fig. 24 provides an upper view while Fig. 25 provides a more closer view of the same.
  • At least one floating electrode 230 is in mechanical communication with at least one membrane 204. More specifically, the floating electrode 230 is glued to membrane 204 in at least one location 211 .
  • the permeate tube 1602 also functions as the anode 206.
  • the cathode 208 is the outer shell (the outer housing enclosing the entire membrane module).
  • additional feed spacer 231 if needed, are added.
  • additional permeate spacer 208a if needed, are added.
  • At least a portion of one face of the floating electrode 230 functions as a cathode (where Hydrogen is produced); and, at least a portion of one face of the floating electrode 230 functions as an anode (where Oxygen is produced). It should be noted that it is within the scope of the present invention where at least one of said floating electrode 230 which functions as a cathode 208 also functions as the permeate spacer.
  • At least one of said floating electrode 230 which functions as an anode 206 also functions as the feed spacer.
  • water production/water filtration is the main product, and less than 1 % of water involved in water purification/desalination process used as source of hydrogen production.
  • water purification/desalination/filtration membranes act in two productions simultaneously and in the same time as a membrane dividing between bipolar and/or mono-polar and/or cathode and/or anode within the same system, in the same time of water purification/desalination.
  • the membrane is in a stack configuration or a spiral configuration.
  • the membrane could be selected from a group consisting of UF, NF, MF, RO membranes and any combination thereof.
  • the electrode e.g., Titanium electrode
  • the spacers could be in addition to the spacers (feed or permeate) or replacing the same (and essentially functioning in the same manner).
  • the spacers are not shown in Fig. 23, it is within the scope of the present invention where the spacers are added or alternatively function as the electrodes (mono or bipolar).
  • Titanium electrode could be in the form of mesh, foil, plate, cloth, fiber, sintered body and any combination thereof.
  • the Titanium electrodes could be at least partially coated with at least one catalyst.
  • the catalyst is selected from a group consisting of iridium oxide, ruthenium oxide, tantalum oxide, titanium oxide, platinum, and platinum oxide, Cobalt, Cobalt oxide, Nickel, Nickel oxide and any combination thereof.
  • At least one of the Titanium electrodes could be at least partially corrugated (as illustrated in Figures 13-14).
  • Figs. 26-27 illustrating another embodiment of the present invention, according to which at least of the spacers (feed and ⁇ or permeate)/electrode are in mechanical communication with each other to one another to form one continuous (elongated) spacer/electrode.
  • the spacers are coupled (e.g., welded, glued or any other means to couple the spacers to one another) to one another to form one continuous (elongated) spacer/electrode.
  • Figs. 26-28 an example is illustrated where several the feed spacer/anode electrodes 206 are coupled to each other at at least one end thereof.
  • the feed spacer/anode electrodes 206 are coupled together (e.g., welded/glue or otherwise joint together) where each one is offset relative to the other.
  • the fist feed spacer/anode electrodes 206 is coupled to the second feed spacer/anode electrodes 206 at a distance 206b from the edges.
  • the third feed spacer/anode electrodes 206 is coupled to the second feed spacer/anode electrodes 206, again, at a distance 206b from the edges.
  • feed spacer/anode electrodes 206 are coupled to each other at a constant distance 206b, at a varying distance 206b or any combination (namely, some at a fixed distance 206b and some are at a changing distance 206b).
  • all the spacers/electrode are coupled to each other to form one continuous (elongated) spacer/electrode.
  • a portion of the spacers/electrode are coupled to each other to form one continuous (elongated) spacer/electrode, while another portion is not.
  • Fig. 28 is a closer view of the assembly of the feed spacer/anode electrodes 206 and the permeate spacer/cathode electrodes 208 (shown in Figs. 26-27).
  • the feed spacer/anode electrodes 206 are welded at one end thereof together, in between two coupled neighboring feed spacer/anode electrodes 206, is place at least one permeate spacer/cathode electrodes 208 and at least one membrane 204.
  • at least one permeate spacer/cathode electrodes 208 and at least one membrane 204 are placed between two neighboring feed spacer/anode electrodes 206 joint together.
  • FIG. 29 illustrating another embodiment of the present invention where both spacers (permeate and feed spacers) and electrodes (Titanium foils) are employed.
  • all anode electrodes 1600a are welded to the permeate tube 1602.
  • the envelope enclosing the permeate spacer 208 and the membrane 204 now includes also at least one anode electrode 1600a (e.g., Titanium foil) and two standard permeate spacers.
  • the cathode electrode e.g., Titanium foil
  • the cathode electrode is positioned in between two feed spacers 206.
  • the electrode could be any of the disclosed above (e.g., at least partially corrugated, in the form of a mesh, with coating of at least one catalyst etc.).
  • hydrogen and oxygen evacuation systems may be applied to remove the gases from the membrane system.
  • hydrogen and oxygen are evacuated from the membrane element or module together with the water stream in which they were generated. Extraction of hydrogen and oxygen may then take place in a degasifier.
  • the solubility of hydrogen and oxygen in water is very different enabling extraction of hydrogen to take place in the degasifier at a pressure at which oxygen is still dissolved.
  • Oxygen together with water stream may then go to next degasifier with a lower gauge pressure, where oxygen may then be extracted.
  • a gas separation membrane may be utilised.
  • the present invention allows fluids produced during treatment of water, such as seawater, brine and brackish water to be electrochemically split to provide hydrogen in addition to the treated water.
  • one RO module may be provided with several membrane elements and feed seawater is concentrated as it moves from one membrane to the next membrane element in the module.
  • the first element in a module may have seawater 3.5% TDS and in the 8 th membrane element 8% TDS.
  • the water electrolysis will be different in different membrane elements having different salinity.
  • the electrical system may be adjusted to provide different electrical current (voltage) to different membrane in module.
  • one RO module contains 5-8 membrane elements.
  • the desalinated permeate stream produced during the RO process is split into hydrogen and oxygen. This provides an important technological benefit in that permeate is never free from dissolved suspended solids.
  • FIG. 7 of the accompanying drawings illustrates a conventional seawater desalination plant that may be adapted to include membranes with electrodes to provide a dual water desalination and hydrogen generation plant.
  • sea water SW is delivered, via intake channel 101 , through various pre-treatment sites 102, 103, 104, 105 before being pumped under pressure by virtue of pumps 108 through multiple reverse osmosis passes 110, 112 to form desalinated product water 1 14 and concentrated sea water or brine 116.
  • the product water may be subjected to posttreatments 118 and held in a holding tank 120, while the brine 1 16 is be discharged back into the sea via a discharge channel 122.
  • the reverse osmosis passes 1 10, 1 12 are each made up of multiple membrane elements 201 , one of which is exemplified and expanded in Figure 7.
  • a central perforated product tube 202 extends through the centre of each element and is surrounded by sheets of semi-permeable membrane 204 wound around the tube and separated therefrom by a feed spacer sheet 206 and a permeate spacer sheet 208.
  • An anti-telescoping cap 210 is provided at each end.
  • a raw saline feed solution is fed into one end of the element 201 to provide permeate stream 114 and residual brine stream 1 16 with a permeate flow PF through the layers of the element.
  • Electrodes can be incorporated within the element to allow electrochemical splitting of raw saline solution and/or permeate to create a smaller output of hydrogen generation (not shown) together with a main output of residual brine stream 1 16 and/or permeate product water 114.
  • the process and system for simultaneous water treatment and electrochemical splitting of water according to the present invention addresses many problems associated with prior art generation of hydrogen from seawater and other water sources.
  • the possibility of cathodic precipitation of CaCOs, Ca(OH) 2 , Mg(OH) 2 and other species in the hybrid reactors proposed by the Applicant for simultaneous water treatment and H 2 production is significantly lower due to (i) very low current density, (ii) very high water flux, and (iii) the pH buffering capacity of seawater (relevant only if cathodes are located in feed and/or in concentrate compartments).
  • FIG. 8 of the accompanying drawings is a graph showing reversible potentials for chlorine evolution, oxygen evolution and hydrogen evolution reactions as a function of pH.
  • T 25°C
  • the electrode potential for anodic reactions must be higher than the reversible potential.
  • the cathode potential must be lower than the reversible potential of this reaction.
  • the minimal cell potential required for oxygen evolution on an anode and hydrogen evolution on a cathode is only 1 .23 Volt. Consequently, there is a range of cell potentials at which only oxygen will be produced on the anode and hydrogen will be produced on a cathode.
  • this maximal cell potential limits the anodic current density to the very low current density of only few mA/cm 2 .
  • the current densities typical for alkaline water electrolysis is 200-400 mA/cm 2 , and 600-2000 mA/cm 2 for PEM water electrolysis and thus, chlorine generation would be a problem.
  • the very small current density applied in the present invention allows chorine generation to be depressed.
  • the proposed technique has the same thermodynamics as the conventional water electrolysis processes.
  • operation at higher current density i.e., larger production rates per reactor volume
  • energy/H 2 ratio increases at higher current densities.
  • very low current densities that will be utilised for the process of the present invention is expected to result in lower electrical energy consumption for hydrogen production compared to the state-of-the-art technologies.
  • the main reasons for this lower energy consumption are as follows: (1 ) lower activation overpotential is required to achieve lower current density, (2) very low diffusion and concentration overpotentials due to very effective mass transport in the proposed systems, (3) gas generation at no formation of bubbles.
  • one of the main requirements to modern water electrolysis processes is low energy consumption at sufficient (i.e., > 200 mA/cm 2 ) current densities.
  • High current density is required to decrease the construction costs, the footprint, and amounts of expensive materials, such as catalysts, membranes, bipolar plates, etc.
  • construction of large conventional water electrolyzer operated at very low current density is economically unfeasible due to very high construction costs that would diminish the benefits of low energy consumption.
  • the integration of a hydrogen-producing process in conventional water desalination/filtration systems according to the present invention is possible without any increase in their size or any significant decrease in water treatment performance.
  • permeate and feed spacers of RO, NF, UF, and FO modules can be used as they currently are for separation of anodes and cathodes incorporated therein to provide the desired hydrogen generation. Consequently, the capital costs of the proposed H 2 production systems are expected to be relatively low, as they utilize materials, water preconditioning systems, and other units that already exist in pressure-driven membrane filtration processes.
  • Conventional water electrolysis electrodes comprise the “real electrode” which is a very thin ( «few microns) layer of catalysts, and secondary layers, such as a gas diffusion layer (GDL).
  • the GDL is used to achieve fast mass transport of gaseous products from the electrode, and to drive electrons to (or from) the electrode.
  • the GDLs of modern PEM water electrolyzers contain hydrophobic particles for fast transport of gaseous species.
  • the current collector is used to provide a flow of electrons to (or from) the GDL and the catalyst layer.
  • the current collectors have flow-fields to distribute water on the electrode surface and to collect the produced gases.
  • the thickness of current collectors is normally > 3 mm and they are made of highly conductive material (e.g., graphite, composite of polymer and conductive particles, or metals).
  • the electrodes of the electrolysis cells proposed by the semi-permeable membranes of the Applicant must be made of conducting fibers which are relatively long (i.e., up to 100 cm inside the membrane) and relatively thin (apparently up to 100 pm). This geometry would be barely possible in conventional WE operated at high current density. This is due to a high resistance of fiber-type electrodes. However, a simple calculation shows that this fiber type geometry is applicable in the systems and processes proposed herein:
  • the cross-sectional current density (the ratio between current and cross-section of fiber electrodes) becomes » 0.6 A/mm 2 .
  • the electrodes have electrical conductivity of 1 .27-105 (S/m) (typical for graphite in basal plane) the ohmic voltage drop in 100 cm long electrode at a current of 30 A will be only » 50 mV.
  • S/m electrical conductivity of 1 .27-105
  • the ohmic voltage drop in 100 cm long electrode at a current of 30 A will be only » 50 mV.
  • This simple calculation shows that the proposed electrochemical cells are feasible if fiber type electrodes are made of material with high electrical conductivity (i.e., within a range of stainless steel or titanium).
  • FIG. 9 of the accompanying drawings illustrate one scheme which may incorporate the system for generating hydrogen as hereinbefore described.
  • the scheme allows for production of green energy using osmotic power generation from salt domes, the energy then being utilised for water split as hereinbefore described followed by storage of the hydrogen in empty salt caverns.
  • the invention provides an extremely energy efficient manner for the production of green energy in the form of hydrogen.
  • the scheme involves 3 cycles; cycle 100 involving efficient energy generation by PRO using the different salt concentrations between sea water 2 and dissolved salt water from salt domes 26; cycle 200 involving hydrogen generation from water electrolysis using the electricity produced in cycle 100 and cycle 300 which evacuates the hydrogen produced in cycle 200 and delivers it for storage in salt dome caverns 35 formed during salt extraction for the PRO in cycle 100.
  • cycle 100 creates electricity using Pressure Retarded Osmosis process (PRO).
  • PRO Pressure Retarded Osmosis process
  • the PRO is driven by the difference in salinity between highly concentrated salt 10-25% (draw solution DS) dissolved from salt domes 26 and seawater 3.6-4.5% (the feed solution FS).
  • the dissolution of salt rock in salt caverns 26 as an option can take place under high gas pressure PGr which can be of about 200 bar and forms the draw solution. Alternatively, the dissolution can take place under atmospheric pressure.
  • This draw solution is delivered to a first PRO module 100 by means of pump 25 via pipe line 23 and enters the first side of the module 100 via inlet 22 the first side.
  • the feed stream (FS) enters the second side of the PRO module 100 via inlet 20.
  • Part of the feed stream penetrates from the second side to the first side of the membrane 3 as low salinity permeate and mixes with the draw solution. A mix of the draw solution and permeate then exit module 100 via outlet 23. Part of this mix is directed to turbine 27 for electricity generation.
  • the residual amount of the feed stream is discharged from module 100 via outlet 21 to environment (for example, the sea as shown in Figure 5)
  • the electricity generated in turbine 27 or similar device from the output from module 100 is then directed to a Forward Osmosis (FO) module 200 as energy source for electrochemical water split into hydrogen and oxygen, with the low salinity water for water split coming from FO process and the water split being achieved by the incorporation of a membrane according to the invention into the module that has electrodes for effecting electrolysis.
  • Sea water 2 may be used for the feed solution 30.
  • Module 200 FO from construction point of view is similar to PRO module 100. Movement of permeate stream from the feed side of membrane to the draw side also takes place under balance of osmotic and gauge pressures Por; Pof; PGr; PGf. However, the difference between modules 100 and 200 is in the gauge pressures PGr; PGf. On module 200 the PGr and PGf are low and permeate movement from the FS side to the DS side takes place mostly under the difference in osmotic pressures Por’ and Pof’.
  • the membrane has electrodes (i.e. 9,10 in Figures 1 A to 4) and optionally an additional reference electrode (not shown in drawings). These electrodes, together with the electricity from module 100, allow splitting of the low salinity permeate stream to take place producing hydrogen and oxygen. Any residual water 33 may be returned to the sea 2.
  • the semi-permeable membranes incorporating electrodes according to the present invention may be installed in module 100 and module 200, thus allowing water split to take place on module 100 and module 200 at the same time.
  • the electrodes can be installed in module 100 only or in module 200 only.

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Abstract

La présente invention concerne de manière générale la production d'une eau dessalée, filtrée ou traitée d'une autre manière simultanément avec la génération d'une source d'énergie renouvelable, en particulier de l'hydrogène, à l'aide de procédés et de systèmes de filtration entraînés par pression osmotique et/ou de jauge. L'invention concerne également la co-génération d'hydrogène 11 à partir de l'eau 8 produite pendant des processus de dessalement/filtration d'eau entraînés par la pression, tels que l'osmose inverse, l'osmose directe, l'osmose retardée par la pression ou l'ultrafiltration. Une petite partie de la solution saline brute et/ou du perméat d'alimentation impliquée dans des processus de dessalement/filtration est soumise à une électrolyse, divisant ainsi l'eau pour produire de l'hydrogène. Ceci est obtenu par la fourniture de nouvelles membranes semi-perméables de type RO et d'une membrane de type UF qui incorporent des électrodes 9, 10 à l'intérieur de la membrane pour permettre la division de l'eau par électrolyse.
PCT/IB2024/058000 2021-12-29 2024-08-17 Source d'énergie renouvelable utilisant des processus et des systèmes de filtration entraînés par la pression Pending WO2025041021A1 (fr)

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US202463618253P 2024-01-05 2024-01-05
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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20150321929A1 (en) * 2012-12-02 2015-11-12 Axine Water Technologies Inc. Method for imparting filtering capability in electrolytic cell for wastewater treatment
US20230032928A1 (en) * 2019-12-26 2023-02-02 Vito Nv Method for generating hydrogen and oxygen from a liquid feed stream comprising water, and device therefor
WO2023126881A1 (fr) * 2021-12-29 2023-07-06 IDE Water Technologies Ltd Source d'énergie renouvelable utilisant des processus et des systèmes de filtration entraînés par la pression

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20150321929A1 (en) * 2012-12-02 2015-11-12 Axine Water Technologies Inc. Method for imparting filtering capability in electrolytic cell for wastewater treatment
US20230032928A1 (en) * 2019-12-26 2023-02-02 Vito Nv Method for generating hydrogen and oxygen from a liquid feed stream comprising water, and device therefor
WO2023126881A1 (fr) * 2021-12-29 2023-07-06 IDE Water Technologies Ltd Source d'énergie renouvelable utilisant des processus et des systèmes de filtration entraînés par la pression

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