WO2021126073A1 - Cellule électrolytique à membrane et procédé d'utilisation - Google Patents

Cellule électrolytique à membrane et procédé d'utilisation Download PDF

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Publication number
WO2021126073A1
WO2021126073A1 PCT/SG2019/050630 SG2019050630W WO2021126073A1 WO 2021126073 A1 WO2021126073 A1 WO 2021126073A1 SG 2019050630 W SG2019050630 W SG 2019050630W WO 2021126073 A1 WO2021126073 A1 WO 2021126073A1
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WO
WIPO (PCT)
Prior art keywords
water
membrane
electrolytic
hydrogel membrane
electric circuit
Prior art date
Application number
PCT/SG2019/050630
Other languages
English (en)
Inventor
Qipeng ZHAO
King Kheng WONG
Beng Tiong Lim
Original Assignee
International Renewal Energy Holding Pte. Ltd.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by International Renewal Energy Holding Pte. Ltd. filed Critical International Renewal Energy Holding Pte. Ltd.
Priority to AU2019478718A priority Critical patent/AU2019478718A1/en
Priority to CN201980103569.1A priority patent/CN115279947A/zh
Priority to PCT/SG2019/050630 priority patent/WO2021126073A1/fr
Publication of WO2021126073A1 publication Critical patent/WO2021126073A1/fr

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Classifications

    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25BELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B1/00Electrolytic production of inorganic compounds or non-metals
    • C25B1/01Products
    • C25B1/02Hydrogen or oxygen
    • C25B1/04Hydrogen or oxygen by electrolysis of water
    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25BELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B13/00Diaphragms; Spacing elements
    • C25B13/02Diaphragms; Spacing elements characterised by shape or form
    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25BELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B13/00Diaphragms; Spacing elements
    • C25B13/04Diaphragms; Spacing elements characterised by the material
    • C25B13/08Diaphragms; Spacing elements characterised by the material based on organic materials
    • CCHEMISTRY; METALLURGY
    • C25ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25BELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/70Assemblies comprising two or more cells
    • C25B9/73Assemblies comprising two or more cells of the filter-press type
    • C25B9/77Assemblies comprising two or more cells of the filter-press type having diaphragms
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30Hydrogen technology
    • Y02E60/36Hydrogen production from non-carbon containing sources, e.g. by water electrolysis
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30Hydrogen technology
    • Y02E60/50Fuel cells
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02PCLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P20/00Technologies relating to chemical industry
    • Y02P20/10Process efficiency
    • Y02P20/129Energy recovery, e.g. by cogeneration, H2recovery or pressure recovery turbines

Definitions

  • the present invention relates to the field of electro-chemistry, particularly electrolysis.
  • the invention relates to an electrolytic method for gas production.
  • an electrolytic device for use in gas synthesis.
  • the present invention is suitable for use in water splitting.
  • the electrolyser used for water splitting electrolysis is well known in the prior art and typically comprises two electrodes separated by a membrane and immersed in water. Salts may be added to the water to increase electrical conductivity. Passage of an electric current across the electrodes causes water to be reduced by the supply of electrons from the cathode and hydrogen gas is formed. A corresponding oxidation reaction occurs at the anode to generate gaseous oxygen.
  • Liquid polymers have been used as electrolytes in batteries for many decades, but hydrogels are far less utilised. In the past, some efforts have been made to use hydrogels in batteries and fuel cells as electrolytes. For example, alkaline hydrogel electrolytes have been produced by physical cross-linking using poly(vinyl alcohol) and potassium hydroxide and used in a dual role - as electrolyte and barrier in Ni-MH cells. (Osinska-Broniarz et al., Chemik 2015, 69, 12, 852-861).
  • Hydrogels have also been used as membrane electrolytes in application such as fuel cells.
  • direct borohydride fuel cells have been constructed with polymer electrolyte membranes consisting of ionically cross-linked chitosan hydrogel.
  • polymer electrolyte membranes consisting of ionically cross-linked chitosan hydrogel.
  • the prior art typically teaches carrying out water electrolysis reactions in the vapour phase using liquid electrolyte or solid-oxide electrolyte cells.
  • the technology of vapour electrolysis cells is at an advanced stage.
  • hydrogel electrolyte or hydrogel cells are not taught by the prior art as being suitable for water electrolysis.
  • Hydrogel materials have instead been of interest for supercapacitor and rechargeable battery applications because their structures consist of a cross-linked network of polymer chains having interstitial spaces filled with solvent water. Hydrogels are thus both wet and soft, making them ideal candidates for electrolyte materials in flexible energy storage devices, and rechargeable batteries. These uses are reviewed for example in prior art document, Hydrogel Electrolytes for Flexible Aqueous Energy Storage Devices (Wang et al., Adv. Functional Materials 2018, 28, 1804560).
  • An object of the present invention is to provide a membrane electrolyser and method of electrolysis for gas synthesis.
  • a further object of the present invention is to improve the efficiency of electrolytic reactions used for synthesis.
  • a further object of the present invention is to alleviate at least one disadvantage associated with the related art.
  • an electrolytic cell having an electric circuit comprising an anode and a cathode separated by a hydrogel membrane, wherein the hydrogel membrane comprises a hydrophilic polymer and acts as an electrolyte.
  • water absorbed by the polymer is electrolysed when an electric current passes through the electric circuit.
  • a method of electrolysis comprising the steps of; locating a hydrogel membrane comprising a hydrophilic polymer between an anode and a cathode of an electric circuit, absorbing liquid into the hydrogel membrane, passing an electric current through the electric circuit.
  • a method of electrolysis of water comprising the steps of; locating a hydrogel membrane comprising a hydrophilic polymer between an anode and a cathode of an electric circuit, absorbing water into the hydrogel membrane, passing an electric current through the electric circuit such that the water in the hydrogel membrane is reduced to hydrogen at the cathode and oxygen forms at the anode.
  • the gas produced at the electrodes diffuses out of the cell via the polymer membrane, separating the gas from the reaction at the electrode.
  • the gas is separated without significant bubble formation on the electrode. Avoiding bubble formation permits reactions such as water splitting to be achieved with a low over-potential, thereby contributing to the efficiency of the electrolytic cell.
  • the hydrogel membrane preferably comprises a hydrophilic polymer which can absorb a large proportion of water very rapidly and has a robust physical structure.
  • a hydrogel is a macromolecular polymer gel which can hydrogen-bond molecules of water within interstices located throughout a network of crosslinked polymer chains.
  • the water content in the polymer membrane can be as high as 98 wt% of the polymer, but typically the water content is at least 80 wt%, preferably at least 90 wt%.
  • the electrolytic splitting is effectively carried out in a hydrogel environment.
  • the membrane has sufficient mechanical strength to withstand compression pressure of up to 50 bar, preferably more, without substantial alteration in performance.
  • Hydrophilic polymers typically include charged functional groups.
  • the hydrophilic polymer of the present invention is chosen from the group comprising acrylic acid, acrylamide, maleic anhydride, polyacrylic acid, polyacrylamide, polyvinyl alcohol polymers and copolymers thereof.
  • the membrane may comprise one or more polymers.
  • the main composition of the membrane is preferably the product of a copolymer of poly(sodium acrylate-co-acrylamide) with some other ingredients to reinforce the mechanical strength or tune the hydrophilicity.
  • the membrane is formed from reaction of a copolymer of poly(sodium acrylate-co-acrylamide) with N,N’- methylenebisacrylamide crosslinker.
  • a number of water management strategies can be used to ensure constant hydration of the polymer membrane at a desired level.
  • the desired level of water can be calculated by a simple mathematical model based on parameters such as temperature, voltage and current of the electric circuit, or hydrogen flow output.
  • the membrane is hydrated by circulating liquid water through the cell or by introducing water vapour to the polymer membrane.
  • Other suitable hydration methods may also be used.
  • European patent 2 463 407 (Astrium GmbH, corresponding to US 13/991 ,648) describes pumping water into microchannels in a hydrophobic membrane.
  • US patent 2014 0224668 (Jehle et al.) describes a hydrophobic membrane for electrolytic water splitting, the membrane being supplied with liquid water in a passive manner from a reservoir, without using a pump. Water from the reservoir may pass by capillary effect via at least one cavity structure in the membrane.
  • an electrolytic system may be formed according to the present invention, comprising a plurality of electrolytic cells according to the present invention, the electrolytic cells being connected.
  • Each electrolytic cell may have separate or common water feeds.
  • single electrolytic cells of the present invention can be stacked in a manner well known in the prior art to increase the power capacity or hydrogen generation.
  • the present invention therefore further provides an electrolytic system comprising a plurality of electrolytic cells according to the present invention, the electrolytic cells being arranged in a stack such that each electrolytic cell is in electrical connection with at least one adjacent electrolytic cell.
  • the polymer membrane can be made by any convenient means known in the art for constructing membranes, such as polymer moulding or phase inversion techniques.
  • the polymer precursor in liquid/semi-liquid form is injected into customized stainless steel or ceramic moulds.
  • the polymer is then subjected to a predetermined process at desired temperatures, pressures and cycle times.
  • a polymeric membrane is cast onto a uniform substrate material. This is done by phase inversion - a process in which a liquid polymer dope is cast on the substrate material, then passed into a coagulation bath comprising a quenching solution where solvents are drawn out.
  • the catalyst may be supplied in any convenient form, such as a mesh.
  • the electrolytic cell of the present invention may additionally comprise a catalyst associated with the hydrophilic polymer membrane.
  • the catalyst for example, may be deposited upon the porous membrane.
  • precious metals such as platinum, gold or palladium are used for water splitting.
  • the electrolytic cell and method of the present invention may be used in association with less expensive and non-precious catalysts, such as nickel and manganese-based catalysts.
  • the present invention may include incorporation of different catalysts and different chemical reactions when for production of compounds other than hydrogen and oxygen. This could include, for example ammonia (from water and atmospheric nitrogen) or methane, methanol, ethanol, formic acid, or acetic acid from water and carbon dioxide.
  • the electrolytic cell and method of the present invention is used for synthesis.
  • the cell forms part of a fuel cell system.
  • the electrolytic cell of the present invention cannot be applied in the reverse reaction (that is, in a fuel cell reaction) however, it could be integrated into a fuel cell system.
  • the electrolysis cell of the present invention could be used to produce hydrogen by the water splitting reaction, and the hydrogen produced could be stored in a storage tank.
  • Fuel cells could use the hydrogen to provide power to an appliance, such as a car.
  • the electrolytic cell and method of the present invention may be used for water splitting to synthesise hydrogen and oxygen, but it will be readily apparent to the person skilled in the art that other gases could be synthesised.
  • gases could be synthesised.
  • ammonia could be synthesised from nitrogen/water or methane
  • methanol or ethanol could be synthesised from carbon dioxide/water absorbed by the hydrogel membrane.
  • Production of ammonia may be achieved for example, by a two-step reaction process wherein a first electrolytic cell generates hydrogen from water and supplies this hydrogen to a second cell (with a different catalyst) to combine the hydrogen electrochemically with nitrogen.
  • embodiments of the present invention stem from the realization that the separation membrane of an electrolytic cell, in addition to separating gasses, may also be a source of reactant.
  • the membrane that separates oxygen and hydrogen formed during electrochemical splitting of water may also be the source of water for the electrochemical splitting.
  • FIG 1 illustrates a fully assembled electrolytic cell according to the present invention
  • FIG 2 illustrates the electrolytic cell of Fig 1 expanded to show each of the components in perspective view
  • FIG 3 illustrates a stack of electrolytic cells according to the present invention.
  • FIG 4 illustrates the stack of electrolytic cells of Fig 3 expanded to show each of the components in perspective view
  • FIG 5 is a plot of Input power (kW) against hydrogen output (Nm 3 h 1 ) for a stack of 100 electrolytic cells as depicted in FIG 1. LIST OF PARTS
  • the present invention provides a novel system for solid/semi-solid state water splitting, since hydrogels may be considered to be solid or semi-solid materials due to the fact that they behave more like a solid than a liquid.
  • a hydrogel membrane comprising a hydrophilic polymer is used as a solid/semi-solid membrane and electrolyte in one.
  • the hydrogel membrane separates gasses produced by electrolytic reaction while simultaneously providing a source of water for generation of hydrogen and oxygen. Furthermore, by contrast with the prior art, water splitting electrolysis is not performed in the vapour phase.
  • FIG 1 illustrates a fully assembled electrolytic cell (1) according to the present invention.
  • FIG 2 illustrates the electrolytic cell (1 ) of Fig 1 expanded to show each of the components.
  • the electrolytic cell (1) comprises the following sequence of components to form a separate electrically conductive assembly: Ni mesh electrode (catalyst) (4) / hydrogel polymer membrane (6) / Ni mesh electrode (catalyst) (8) / Al corrugated plate (12) / stainless steel corrugated mesh (14).
  • This view also reveals structural elements such as a printed and cured gasket (2) approximately 0.1 mm thick and a polymer frame, preferably a polypropylene frame (10) serves as a support and facilitates assembly of the cell components.
  • structural elements such as a printed and cured gasket (2) approximately 0.1 mm thick and a polymer frame, preferably a polypropylene frame (10) serves as a support and facilitates assembly of the cell components.
  • FIG 3 illustrates ten electrolytic cells (20) of the type shown in FIG 1 and FIG 2 assembled into a stack of ten. All the electrolytic cells (20) are connected in series. There are two copper current collectors (19) at either end of the stack. The electric charge passes from one copper current collector (19) though all subsequent cells (20) in the system to the copper current collector (19) at the other end of the stack, facilitating the electrolysis reaction.
  • the stainless steel corrugated mesh (14) in one electrochemical cell is in close contact with Ni mesh electrode (catalyst) (4) in the adjacent cell to allow electric charge to pass through the system. Both the aluminium plate (12) and stainless steel mesh (14) close the entire system electrically and allow for a charge to flow through from one copper collector (19) to the other thus facilitating the electrolytic reaction.
  • a stainless steel plate replaces the aluminium plate.
  • the hydrogel membranes (6) must be kept hydrated. Water in the hydrogel is typically replenished either by supplying liquid water through the electrolyser channels or by supplying water vapour through special inlet holes on one side (30) of the electrolyser cells.
  • the other side (31) of each of the electrolyser cells may have holes to remove the excess water vapour as well as oxygen produced by the electrolytic reaction.
  • the water may, for example, be pumped or supplied in a passive manner from a reservoir or by any other method known in the art.
  • the holes may also be used for removal of gas - particularly oxygen - generated during the electrolytic process
  • the cell of the present invention is configured such that the anode side of the cell where oxygen is produced is a so-called open cell that allows oxygen to be easily removed.
  • This configuration simplifies the system and associated processes, however it tends to present some difficulties with respect to oxygen collection.
  • FIG 3 The concept of an open anode cell is illustrated at FIG 3.
  • the water vapour inlet side of the cell (30) is at the bottom and vapour flows in the direction of the arrow, excess water vapour mixed with generated hydrogen exiting from outlets on the other side (31 ).
  • the excess water vapour leaves one stack and enters the next stack where it is used.
  • FIG 4 illustrates the stack (26) of electrolytic cells of Fig 3 expanded to show each of the components in perspective view.
  • Fasteners (16 nominally M10 screws, pass through the edges of all elements at their edges to ensure proper sealing of the stack (26).
  • the thick stainless steel end plates (18, 24) located at either end of the stack may be used to collect gas - particularly hydrogen gas - generated during the electrolytic process.
  • the screws (16) are tightened to ensure that pressure evenly distributes across the stack (26).
  • Individual electrolytic cells (20) - ten in this example - are located between the end plates (18, 24).
  • Plastic pipes (22) are also located at the edges of the electrolytic cells (20) to insulate the fasteners from the electrodes and other metal components of the stack (26) fasteners.
  • FIG 5 is a plot of Input power (kW) against hydrogen output (Nm 3 lr 1 ) for a stack of 100 electrolytic cells as depicted in FIG 1 .
  • the 12-kW system formed by the 100-cell stack has a power consumption of 3.6 to 4.4 kWh/Nm 3 depending on the operation mode and applied power. The measurement was repeated three times to generate the three lines.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Inorganic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Manufacture Of Macromolecular Shaped Articles (AREA)

Abstract

La présente invention concerne une cellule électrolytique ayant un circuit électrique comprenant une anode et une cathode séparées par une membrane d'hydrogel, et un système électrolytique comprenant une pluralité des cellules électrolytiques. La membrane d'hydrogel peut comprendre un polymère hydrophile et agit en tant qu'électrolyte. L'invention concerne également un procédé d'électrolyse et un procédé d'électrolyse de l'eau. Le procédé peut comprendre la localisation d'une membrane d'hydrogel comprenant un polymère hydrophile entre une anode et une cathode d'un circuit électrique, l'absorption de liquide dans la membrane d'hydrogel, et le passage d'un courant électrique à travers le circuit électrique. Le liquide peut être de l'eau. Pour le procédé d'électrolyse de l'eau, le passage du courant électrique à travers le circuit électrique peut être tel que l'eau dans la membrane d'hydrogel est réduite en hydrogène au niveau de la cathode et que de l'oxygène se forme au niveau de l'anode.
PCT/SG2019/050630 2019-12-20 2019-12-20 Cellule électrolytique à membrane et procédé d'utilisation WO2021126073A1 (fr)

Priority Applications (3)

Application Number Priority Date Filing Date Title
AU2019478718A AU2019478718A1 (en) 2019-12-20 2019-12-20 Membrane electrolysis cell and method of use
CN201980103569.1A CN115279947A (zh) 2019-12-20 2019-12-20 膜电解池及其使用方法
PCT/SG2019/050630 WO2021126073A1 (fr) 2019-12-20 2019-12-20 Cellule électrolytique à membrane et procédé d'utilisation

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
PCT/SG2019/050630 WO2021126073A1 (fr) 2019-12-20 2019-12-20 Cellule électrolytique à membrane et procédé d'utilisation

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WO2021126073A1 true WO2021126073A1 (fr) 2021-06-24

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WO (1) WO2021126073A1 (fr)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20200240028A1 (en) * 2017-10-17 2020-07-30 Fujifilm Corporation Water splitting device
CN113088986A (zh) * 2021-02-25 2021-07-09 四川大学 基于聚电解质凝胶海水原位自捕集制氢装置、系统及方法
WO2022006640A1 (fr) * 2020-07-10 2022-01-13 Fortescue Future Industries Pty Ltd Cellule d'électrolyse et procédé d'utilisation
WO2022077064A1 (fr) * 2020-10-14 2022-04-21 Fortescue Future Industries Pty Ltd Membrane pour la génération d'hydrogène et son procédé de formation

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2005307232A (ja) * 2004-04-19 2005-11-04 Mitsubishi Electric Corp 水電解装置及びその運転方法
US20140202875A1 (en) * 2011-02-03 2014-07-24 Ceram Hyd Electrolyser and assembly comprising same, in particular for the production of h2 and o2
CN106757130A (zh) * 2017-01-03 2017-05-31 东南大学 一种胶体电解质膜以及电解水装置

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2005307232A (ja) * 2004-04-19 2005-11-04 Mitsubishi Electric Corp 水電解装置及びその運転方法
US20140202875A1 (en) * 2011-02-03 2014-07-24 Ceram Hyd Electrolyser and assembly comprising same, in particular for the production of h2 and o2
CN106757130A (zh) * 2017-01-03 2017-05-31 东南大学 一种胶体电解质膜以及电解水装置

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US20200240028A1 (en) * 2017-10-17 2020-07-30 Fujifilm Corporation Water splitting device
WO2022006640A1 (fr) * 2020-07-10 2022-01-13 Fortescue Future Industries Pty Ltd Cellule d'électrolyse et procédé d'utilisation
WO2022077064A1 (fr) * 2020-10-14 2022-04-21 Fortescue Future Industries Pty Ltd Membrane pour la génération d'hydrogène et son procédé de formation
CN113088986A (zh) * 2021-02-25 2021-07-09 四川大学 基于聚电解质凝胶海水原位自捕集制氢装置、系统及方法

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CN115279947A (zh) 2022-11-01
AU2019478718A1 (en) 2022-08-18

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