EP4150689A2 - Système de pile à combustible - Google Patents

Système de pile à combustible

Info

Publication number
EP4150689A2
EP4150689A2 EP21726616.2A EP21726616A EP4150689A2 EP 4150689 A2 EP4150689 A2 EP 4150689A2 EP 21726616 A EP21726616 A EP 21726616A EP 4150689 A2 EP4150689 A2 EP 4150689A2
Authority
EP
European Patent Office
Prior art keywords
fuel cell
air
cathode
cell system
line
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
EP21726616.2A
Other languages
German (de)
English (en)
Inventor
Oliver Harr
Philipp Hausmann
Benjamin Pieck
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Cellcentric GmbH and Co KG
Original Assignee
Cellcentric GmbH and Co KG
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 Cellcentric GmbH and Co KG filed Critical Cellcentric GmbH and Co KG
Publication of EP4150689A2 publication Critical patent/EP4150689A2/fr
Pending legal-status Critical Current

Links

Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04223—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids during start-up or shut-down; Depolarisation or activation, e.g. purging; Means for short-circuiting defective fuel cells
    • H01M8/04225—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids during start-up or shut-down; Depolarisation or activation, e.g. purging; Means for short-circuiting defective fuel cells during start-up
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H01M8/04097—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with recycling of the reactants
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H01M8/04111—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants using a compressor turbine assembly
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H01M8/04119—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying
    • H01M8/04126—Humidifying
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H01M8/04119—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying
    • H01M8/04156—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying with product water removal
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
    • H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
    • H01M8/04119—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying
    • H01M8/04156—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying with product water removal
    • H01M8/04164—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants with simultaneous supply or evacuation of electrolyte; Humidifying or dehumidifying with product water removal by condensers, gas-liquid separators or filters
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04223—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids during start-up or shut-down; Depolarisation or activation, e.g. purging; Means for short-circuiting defective fuel cells
    • H01M8/04231—Purging of the reactants
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04223—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids during start-up or shut-down; Depolarisation or activation, e.g. purging; Means for short-circuiting defective fuel cells
    • H01M8/04253—Means for solving freezing problems
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/043—Processes for controlling fuel cells or fuel cell systems applied during specific periods
    • H01M8/04302—Processes for controlling fuel cells or fuel cell systems applied during specific periods applied during start-up
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04313—Processes for controlling fuel cells or fuel cell systems characterised by the detection or assessment of variables; characterised by the detection or assessment of failure or abnormal function
    • H01M8/04664—Failure or abnormal function
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04694—Processes for controlling fuel cells or fuel cell systems characterised by variables to be controlled
    • H01M8/04791—Concentration; Density
    • H01M8/04798—Concentration; Density of fuel cell reactants
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
    • H01M8/04298—Processes for controlling fuel cells or fuel cell systems
    • H01M8/04694—Processes for controlling fuel cells or fuel cell systems characterised by variables to be controlled
    • H01M8/04955—Shut-off or shut-down of fuel cells
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M2008/1095—Fuel cells with polymeric electrolytes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the invention relates to a fuel cell system according to the preamble of claim 1. It also relates to a method for operating such a fuel cell system.
  • Fuel cell systems with at least one fuel cell stack are known so far from the prior art. For example, they can be used to generate electrical drive power in vehicles.
  • the fuel cells in particular for this purpose, are typically so-called PEM fuel cells, that is to say low-temperature fuel cells with a membrane that is permeable to protons.
  • PEM fuel cells that is to say low-temperature fuel cells with a membrane that is permeable to protons.
  • This type of fuel cell is now relatively common. However, it has two serious problems with regard to its service life in regular operation. On the one hand, this is the constant need to keep the membranes sufficiently moist during operation, since drying out of the membranes can significantly shorten the service life of the fuel cells.
  • Another problem is primarily associated with the supply of fuel and oxygen, typically hydrogen and atmospheric oxygen, to the fuel cells during start-up.
  • An exemplary fuel cell system can be found in DE 102009 043 569 A1.
  • This system provides on the one hand a system bypass for connecting the pressure side with the exhaust air side on the one hand and on the other hand a connection between the anode side and the cathode side via a blow-off line with a so-called blow-off or purge valve.
  • a gas / gas humidifier that is customary in such fuel cell systems is indicated, which is used to humidify the supply air flow to the cathode compartment of the fuel cell by means of its humid exhaust air flow.
  • these components are relatively large, complex and expensive.
  • the object of the present invention is to provide an improved fuel cell system which, due to its structure, can dispense with a gas / gas humidifier and avoid numerous operating situations that impair the safety and service life of the fuel cell.
  • the fuel cell system comprises at least one fuel cell stack, which in turn comprises an anode compartment and a cathode compartment.
  • the fuel cell stack can preferably be constructed as a PEM fuel cell stack from a multiplicity of individual cells. It is also known collectively as a fuel cell or fuel cell stack.
  • the cathode compartment of this fuel cell is supplied with air via a supply air line via at least one air delivery device. The air then escapes through an exhaust duct the cathode compartment, for example, into the environment.
  • at least one fuel supply device is provided for supplying the anode space with fuel. This can, for example, be a compressed gas storage device for hydrogen as fuel.
  • the structure of the fuel cell system will also typically have what is known as an anode circuit, which is used to recirculate unused fuel, in particular hydrogen. This is recirculated around the anode compartment, i.e. returned from the exit of the anode compartment to the entrance. In most operating situations, it is mixed with fresh hydrogen and fed back into the anode compartment.
  • the fuel cell system also includes a cathode bypass, that is to say, for example, a line which is formed parallel to the cathode.
  • this cathode bypass branches off in front of or in the area of a valve device in the supply air line and opens into the exhaust air line after or in the area of a further valve device. All of this can be built up on the system side around the cathode compartment or the fuel cell. However, it can also be fully or partially integrated into the fuel cell and / or its housing.
  • the cathode compartment can thus be shut off and the air actually flowing into the cathode compartment and flowing through it can be guided through the cathode bypass.
  • Mixed forms of these two operating states are conceivable, possible and often also useful.
  • a gas jet pump driven by the air flowing around the cathode space is arranged in the cathode bypass.
  • the gas jet pump is thus driven by this air as a propulsion jet in the event that air is passed around the cathode space.
  • the gas jet pump is connected to both the anode compartment and the cathode compartment in a switchable manner on the suction side.
  • a fan in the anode circuit is driven as a recirculation conveying device by an exhaust air turbine in the exhaust air line.
  • energy in the exhaust air can thus be used.
  • this energy should not be used in an electric turbocharger to support the compression of the supply air, but rather to recirculate the anode exhaust gases in the anode circuit. This then enables, for example, an efficient exhaust gas recirculation despite the use of the energy contained in the exhaust air, which will be explained in more detail later.
  • valve devices in the supply air line and / or exhaust air line, in the area of which the cathode bypass branches off can, according to a very advantageous embodiment, each be designed as 3/2-way valves. In principle, a different design or just a 3/2-way valve and a shut-off valve in the other line would also be conceivable. In principle, it should only be ensured that the volume contained in the cathode space can be shut off while the air flows through the cathode bypass with the gas jet pump.
  • the air delivery device used in the fuel cell system according to the invention can preferably be designed in two stages.
  • a sufficiently high pressure can be achieved in order to be able to operate the gas jet pump in the cathode bypass very efficiently.
  • any type of two-stage compression is conceivable, for example by means of two electrically driven flow compressors connected in series.
  • the two-stage air delivery device is designed in the form of a free-running turbocharger, which is connected on the turbine side to the pressure side of a first compressor wheel of an air compressor, and which on the compressor side is connected to the pressure side of a second compressor wheel of the same air compressor is.
  • the air compressor in the fuel cell system according to the invention according to this embodiment thus has two compressor wheels which, according to an extremely favorable further development of this embodiment, are symmetrical and are arranged on a shaft with a common electric motor. This enables a structure in which the symmetrical arrangement of the compressor wheels and the electrical drive arranged in between enables a very good compensation of axial forces. This increases the efficiency, since the friction can be minimized.
  • the electrically driven flow compressor provides a pressure level of 1.5 to 2.5 bar on the first compressor wheel, then this pressure can be increased further via the freewheel, for example up to 4.5 bar to supply the fuel cell.
  • the structure also makes it possible to supply the fuel cell system with very humid gases, since the structure of the freewheel can be designed in such a way that, in the event that it freezes, it still allows sufficient air from the first electrically driven compressor wheel to pass through, as does the fuel cell system to be able to start in adverse weather conditions.
  • a water separator is arranged in the exhaust air line in the flow direction of the exhaust air after the opening of the cathode bypass into the exhaust air line. In this way, the water that occurs in the area of the cathode compartment during regular operation can be separated and collected in this water separator. Since most of the product water accumulates in the area of the cathode compartment, this is the primary amount of water accumulated in the fuel cell system.
  • the water from this area of the fuel cell system reaches the cathode bypass and from here into the Water separator in the exhaust line. This therefore collects all of the water in the fuel cell system.
  • a turbine for driving a fan as a recirculation conveying device is arranged in the exhaust air line, it can also be provided that the water separator is located in the flow direction in front of this exhaust air turbine. In this way, it can protect the exhaust air turbine from droplets that are potentially contained in the exhaust air and which could possibly damage the high-speed turbine.
  • An extremely favorable embodiment of the fuel cell system according to the invention can also provide that an exhaust gas recirculation line connects the exhaust air line after the opening of the cathode bypass and, if an exhaust air turbine is provided, also after this with a register line between the two compression stages.
  • This structure allows exhaust gas recirculation in order to return exhaust air and in particular the moisture contained in the exhaust air to the cathode compartment.
  • the second compressor stage in particular the free-running turbocharger, can thus be used for the recirculation of exhaust air, which is now wholly or preferably partially recirculated and circulated through the second compressor stage, in particular the free rotor.
  • the moisture which is carried along in the cathode exhaust air as a product of the reaction in the fuel cell and which has not already been separated out in the form of liquid water, if a water separator is provided, can be returned.
  • the supply air to the cathode compartment can be humidified and, on the other hand, the oxygen content in the supply air to the cathode compartment can be reduced, in particular adjusted.
  • the oxygen content in the cathode can be reduced. In this way, excessively high cell voltages and thus damage to the individual cells of the fuel cell can be prevented. This procedure is also known as oxygen depletion or air starvation.
  • the fuel cell system according to the invention can have a liquid water system. At least one water separator is connected to a water tank or forms it directly. The water tank itself is then connected to a pressure water distributor, for example a common rail, via a water pump. Branch lines to consumption points for the liquid water then branch off from this pressurized water distributor.
  • the liquid water can advantageously be heated, for example by means of waste heat from the fuel cell system or also by means of electrical heating.
  • Such components are also used in the Combustion engines are used so that they are easily and cost-effectively available on the market.
  • the consumption points include hydrodynamic bearings of the free-running turbocharger and / or at least one humidifier in the supply air.
  • This humidifier can in particular be designed in the form of a one-fluid or two-fluid nozzle.
  • the liquid water system therefore allows the freewheeler, if it is available, to be stored hydrodynamically.
  • the humidifiers can now be designed in a particularly simple manner in the form of a one-fluid or two-fluid nozzle. These humidifiers can be arranged in the supply air before and / or after the second compressor stage. As a result, the compression by the injected water, for example finely atomized water from a two-substance nozzle, is correspondingly moist and is atomized in the two-substance nozzle by the air flowing around the actual water nozzle. This atomized water helps to cool the air that becomes hot during compression and is evaporated in the air so that it is ideally humidified. In particular with an electric drive of the corresponding humidifier, humidification can take place independently of the operation of the fuel cell, which is another very decisive advantage compared to a much more complex, larger and more expensive gas / gas humidifier, which can be saved by this structure.
  • the fuel cell system in one or the other embodiment according to the invention now shows its particular advantages when it comes to achieving corresponding advantages by operating the gas jet pump in the cathode bypass and in particular to avoid adverse operating conditions for the service life of the fuel cell.
  • the method according to the invention therefore provides that, if necessary, the cathode compartment and / or the anode compartment are connected to the gas jet pump and gases are thus sucked out of these areas.
  • this can be used, for example, to support air starvation, which can be initiated primarily via the exhaust gas or exhaust air recirculation, if necessary, especially in system states in which there is no sufficient oxygen-depleted exhaust air available for recirculation.
  • Another aspect can be used, for example, to increase the safety of the fuel cell system when it is used in a vehicle.
  • the anode compartment is still filled with hydrogen and the cathode compartment is still filled with oxygen, a correspondingly high voltage will be applied to the fuel cell, which can be problematic for both the occupants and any rescue workers.
  • the compressor and turbocharger if present, are still active at the time of the accident. If the vehicle's crash sensors detect an accident, the hydrogen supply can be interrupted and the flow through the cathode compartment blocked via the valves.
  • Another very favorable possibility of using the fuel cell system according to the invention is when preparing for a later start of freezing. Because the anode and the cathode can be sucked off via the gas jet pump in the cathode bypass, the pressure in the fuel cell stack can be lowered, preferably evenly, both in the anode compartment and in the cathode compartment. A pressure reduction to, for example, up to 100 mbar is possible. In practice, this means that water, which is in liquid form in the fuel cell and there, due to the risk of later freezing if the Temperatures dropping below freezing point, is not desirable, is already vaporized at very low temperatures of 20 to 40 °, in particular 25 to 30 ° C.
  • the membranes can also be humidified at a standstill if required.
  • liquid water available in the fuel cell system is metered into the fuel cell system via the humidifier, which can be designed, for example, in the form of an electrically driven injector with a single-fluid nozzle, and is brought to the membranes by inflowing air into the cathode compartment, which is (re) humidified as a result can.
  • Another procedural advantage is that the initially mentioned harmful air / air starts of the fuel cell can be prevented.
  • One possible solution with the fuel cell system according to the invention provides that a vacuum is drawn at least for the cathode compartment and possibly also wholly or partially on the anode, so that the pressure difference typically remains less than 500 mbar. As a result, oxygen is sucked out in the area of the cathode. This process can be repeated from time to time, for example every 10 hours, or at least again when it has been recognized that the start of the fuel cell system is now imminent, similar to the previously customary and now no longer required replenishment of hydrogen . If the temperatures are above freezing point, this would in the long run dry out the membranes very much, since the water contained in them evaporates due to the negative pressure.
  • the above-mentioned moistening of the membranes can be carried out from time to time, which has an advantageous effect on the overall service life of the fuel cell system or its fuel cell.
  • circulation around the cathode is also possible. This enables the air in this circuit to be reduced to 0% oxygen.
  • hydrogen can be introduced into the circuit around the cathode until the oxygen is completely consumed. This metering in of hydrogen can take place, for example, via the anode compartment, into which a certain amount of hydrogen is metered and then sucked out again via the gas jet pump in the cathode bypass.
  • the hydrogen is then mixed with the oxygen in the air and can, for example, react on the catalyst of the cathode until the oxygen is completely consumed.
  • this oxygen-depleted air which essentially consists of nitrogen, can flow into the area of the anode space by opening the purge valve.
  • flow can flow through the cathode compartment parallel to the cathode bypass and is then also filled with nitrogen. This enables an extremely gentle start, in which both the anode compartment and the cathode compartment are filled with nitrogen, without the nitrogen having to be carried along and / or (temporarily) stored. Rather, the special configuration of the fuel cell system according to the invention makes it possible to generate this nitrogen in the fuel cell system when required.
  • Another aspect of fuel cell systems is the poisoning of the anode-side catalytic converter with carbon monoxide that occurs during regular operation and increases with the operating time. So far, this has required an occasional air / air start in order to oxidize the carbon monoxide to carbon dioxide with the oxygen introduced and to remove it from the system.
  • the reduction in the service life of the fuel cell must be accepted. As already mentioned several times above, however, such an air / air start should be avoided as far as possible due to the risk of a reduction in the service life of the fuel cell.
  • the fuel cell system constructed according to the invention now enables an extremely gentle procedure here.
  • the fuel cell itself and thus also its anode compartment, which is susceptible to poisoning the catalyst, is, as already described above, via the Using the cathode bypass with the gas jet pump evacuated.
  • oxygen-containing air flows backwards through the gas jet pump into the anode. This can now remain there passively or, preferably, if a recirculation fan is available, can be circulated by this.
  • the catalytic converter can be refreshed and freed from CO impurities, even without an air / air start being necessary.
  • oxygen and carbon dioxide are then sucked out of the anode compartment or the anode circuit.
  • a simple modification in the structure of the fuel cell system results in numerous advantages in terms of process management, so that an extremely efficient and long-lasting fuel cell system can be made available which enables the fuel cell to be operated very gently.
  • the only attached figure shows a possible embodiment of a fuel cell system according to the invention.
  • an air compressor 1 for a fuel cell system 2 is shown.
  • the air compressor 1 essentially consists of an electric drive motor 4, which is arranged on a common shaft 5 with two compressor wheels 6, 7.
  • the compressor wheels 6, 7 are driven by the electric drive motor 4 arranged centrally between them on the shaft 5 and are designed essentially symmetrically. In this way, forces which act on the common shaft 5 in the axial direction are minimized. On the one hand, this helps to reduce friction losses and, on the other hand, allows a simple and efficient design of axial bearings. Air is sucked in by the compressor wheels 6, 7 via two separate or, optionally, a common suction path 8.
  • the air filters that are typically present are not shown here.
  • a common shaft 12 connects the compressor side 10 with a turbine side 13, which is connected to the pressure side of the compressor wheel 7 of the air compressor 1 and is accordingly driven by the air flow from this compressor wheel 7.
  • the turbine side 13 or its turbine After the turbine side 13 or its turbine, the expanded air, which had previously passed from the compressor wheel 7 to the turbine side 13 of the freewheel 11 via a turbine line 14, flows away again.
  • the turbine-side discharge leads via the compressed gas reservoir 26 for hydrogen into the environment.
  • a bypass line 15 with a valve 16 is provided, which enables part of the air that has been compressed via the compressor wheel 7 of the air compressor 1 to be conducted from the turbine line 14 into the register line 9.
  • a higher volume flow of air to the fuel cell system 2 can be achieved.
  • the air flow through the turbine side 13 of the freewheel 11 is correspondingly reduced, so that although a higher volume flow, but a lower pressure in the Fuel cell system 2 is present.
  • the power on the turbine side 13 and thus also the compressor power on the compressor side 10 of the freewheel 11 increases accordingly, while at the same time the volume flow becomes smaller.
  • the direction of flow can also be such that more air flows to the turbine side 13 of the freewheel 11 via the bypass line.
  • all of the air in the air compressor 1 can be used to drive the freewheel 11.
  • the air supply can therefore be controlled via the valve 16 in the bypass line 15. Even if the bypass line 15 with the valve 16 offers particular advantages, it is to be understood here as being purely optional and can in principle also be omitted.
  • the fuel cell system 2 comprises a fuel cell 19, which is typically a stack of individual cells.
  • a fuel cell stack 19 an anode space 20 and a cathode space 21 are indicated by way of example.
  • the cathode chamber 21 is now supplied with air via a supply air line 22 via the air compressor 1 and the free rotor 11.
  • Exhaust air arrives via an exhaust air line 23 to a valve device labeled 24, wherein this valve device 24 could also be referred to as an exhaust gas recirculation valve 24.
  • the exhaust air from the exhaust air line 23 can be wholly or partially returned via an exhaust air return line 25 to the register line 9 via this valve device 24, or via the section of the exhaust air line 23 labeled 23 ‘into the environment.
  • the exhaust air no longer flows through an exhaust air turbine in section 23 ‘.
  • the anode space 20 is supplied with hydrogen from a compressed gas store 26.
  • a compressed gas storage device 26 As an alternative to such a compressed gas storage device 26, other storage possibilities for the hydrogen would also be conceivable, for example cryogenic storage or hydride storage.
  • this hydrogen reaches the anode compartment 20.
  • an anode circuit 28 with a recirculation line labeled 29, in which a water separator 30 can be arranged exhaust gas then returns from the outlet of the anode compartment 20 to its inlet and flows, in most operating states mixed with fresh hydrogen back into the anode compartment 20.
  • the recirculation line 29 can be known per se
  • a recirculation fan 31 can be arranged.
  • a blow-off line 17 with a so-called blow-off valve or purge valve 18 or purge valve is arranged, via which, for example, depending on the time, depending on the hydrogen concentration in the recirculation line 29 or, depending on other parameters, gas is drained from the recirculation line 29, optionally together with water from the water separator 30.
  • the structure with the combination of air compressor 1 and freewheel 11 thus enables optimal operation with a high degree of controllability of pressure and volume flow of the supplied air - especially in combination with the liquid system 34 - a dispensing with a conventional gas / gas humidifier, since the exhaust gas recirculation becomes possible without the risk of the entire air delivery device 1 freezing in the case of temperatures below freezing point.
  • this pressure cannot be used here for the air delivery device 3.
  • valve device 35 in the flow direction upstream of the cathode compartment 21 and a valve device 36 in both the supply air line 22 and the exhaust air line 23, namely here in each case relatively close to the cathode chamber 21 is arranged after the cathode chamber 21 in the flow direction.
  • These valve devices 35, 36 can preferably, and this is how it is shown here, be designed as 3/2-way valves. However, they could essentially also be implemented by independent valve devices which are arranged both in the supply air line 22 and in the exhaust air line 23, and which would also be arranged in a cathode bypass 37.
  • the cathode bypass 37 can be switched via the valve devices 35, 36, to be precise when the cathode compartment 21 is closed or the volume comprising the cathode compartment 21 is closed.
  • the cathode bypass 37 is provided with a gas jet pump 38 which, for example, can be designed in the manner of a Venturi tube.
  • gas jet pump 38 any other type of gas jet pump or ejector or jet pump is also conceivable, as long as through negative pressure effects and / or Pulse exchange can be sucked in by the air flowing around the cathode chamber 21.
  • the gas jet pump 38 On the suction side, the gas jet pump 38 is connected to the blow-off line 17, which can be switched via the purge valve 18 in order to connect the blow-off line 17 to the gas jet pump 38. In this way, liquid and in particular gas can be sucked out of the anode circuit 28 and thus also out of the anode space 20.
  • anode circuit 28 Since the anode circuit 28 is otherwise tight and forms a closed volume when the hydrogen supply is switched off, a negative pressure can be achieved in the anode circuit 28, which is very favorable for the reasons explained below.
  • the gas jet pump 38 is also connected on the suction side via a cathode stub 39 and a cathode suction valve 40 arranged therein to the cathode compartment 21 or to the volume comprising the cathode compartment 21 located between valve devices 35 and 36.
  • the cathode branch line 39 can be arranged both before and after the cathode space 21, that is to say with an opening into the supply air line 22 or the exhaust air line 23. In principle, a direct connection to the fuel cell stack 19 would also be conceivable, but this is technically far more complex than branching off from the corresponding line 22, 23.
  • gas can now be extracted from the cathode compartment with the cathode bypass 37 flowed through by the gas jet pump 38 with the cathode suction valve 40 open 21, which, when the valve devices 35 and 36 are closed, means that a negative pressure can also be generated in the cathode of the fuel cell 19. This will also be explained in more detail later with regard to the particularly advantageous use.
  • the already mentioned liquid water system 34 is shown in dashed lines in the figure. It can preferably be filled with water which is recovered from the fuel cell system 2.
  • the fuel cell system 2 typically has the water separator 30 in the recirculation line 29 and another water separator 41 in the area of the exhaust air line 23, and here, if possible, upstream of the exhaust air turbine 32.
  • the water from the water separator 30 arrives via the gas jet pump 38 and the cathode bypass 37 also into the water separator 41.
  • a parallel line from the water separator 30, for example into the water separator 41 or directly into a water tank 42 of the Liquid water system 34 conceivable, in which the entire water of all water separators 30, 41 of the fuel cell system 2 then collects.
  • this water tank 42 is now supplied with heat. In principle, this can involve electrical heating, as is generally known and customary for such water tanks in the area of vehicles with internal combustion engines.
  • waste heat from the fuel cell system 2 can also be used, for example waste heat from the fuel cell 19 itself, or waste heat in the exhaust air, in particular in the exhaust air flowing out of the turbine side 13 of the freewheel 11, which, however, can alternatively be used to heat the compressed gas reservoir 26 could.
  • the water stored in the water tank 42 ideally has a temperature of approx. 80 ° C., the water tank 42 therefore has thermal insulation 44 in order to prevent the water tank 42 from cooling down unnecessarily and quickly.
  • the water from the water tank 42 is then passed via a water pump 45 into a pressurized water distributor 50, for example in the form of a so-called common rail.
  • Individual branch lines then branch off from this pressurized water distributor 50.
  • a first branch line 46 leads to a first humidifier 47. This is designed as a simple humidifier 47 which atomizes the water with a single-fluid nozzle or a two-fluid nozzle.
  • a further humidifier 48 which is constructed in a comparable manner, is optionally provided. This is located in the register line 9 and is supplied with the pressurized water of the pressurized water distributor 50 via a second branch line 49.
  • this previous structure of the liquid water system 34 is also used in internal combustion engine drives, in particular internal combustion engines with gasoline injection.
  • the components such as the water pump 45, the heatable water tank 42 and the humidifiers 47, 48 are therefore available on the market as adequately tested parts in large numbers and accordingly inexpensively.
  • the 54 of the free-running turbocharger 11 is supplied with water so that it is mounted on water.
  • the hydrogen supply can be stopped. With the remaining volume flow when the air compressor 1 and the freewheel 11 are coasting down, gas can then be sucked out of the shut-off cathode space 21 and the anode circuit 28 and thus the anode space 20.
  • the (no-load) voltage of the fuel cell 19 can be reduced very quickly when the load is dropped and the current of the fuel cell 19 is reduced to zero, so as to prevent the occupants of the vehicle and rescue workers from being endangered.
  • the oxygen content in the fuel cell 19 can be reduced in order to limit the cell voltage, for which a corresponding amount of oxygen-depleted exhaust air is returned via the exhaust gas recirculation valve 24 and the exhaust gas recirculation line 25 and also supports the humidification of the supply air. If this is not sufficient, oxygen can also be actively sucked out of the cathode compartment 21 with the cathode suction valve 40 open by leading part of the supply air via the cathode bypass 37 and the gas jet pump 38 in order to reduce the voltage in the individual cells or the voltage of the entire cell To limit fuel cell stack 19 further and more reliably controllable.
  • Two very decisive points for the operation of the fuel cell system 2 relate to a preparation for a freeze start, a so-called FSU (Freeze Start Up) preparation. Because it is possible to lower the pressure in the anode compartment 20 and in the cathode compartment 21, for example to up to 100 mbar, it is possible to evaporate water present in both the anode compartment 20 and in the cathode compartment 21 and to actively suck it off via the gas jet pump 38. This can take place, for example, in a temperature window of 25 to 35 ° C. of the fuel cell 19. In contrast to higher temperatures, the membranes are largely prevented from drying out, so that the fuel cell 19 can be dried very gently.
  • FSU Freeze Start Up
  • the fuel cell can be prevented from freezing beyond an intended or tolerable level. If the temperatures rise again above freezing point, active humidification can be carried out even without the fuel cell 19 being actively started, since liquid water is available via the liquid water system 34 and, for example, via the humidifier 47, which in particular is an electrically operated humidifier can be designed with a single-fluid nozzle, can be easily and efficiently introduced into the supply air. As already mentioned, this can be circulated via the exhaust gas recirculation valve 24, on the one hand to keep the membranes sufficiently moist and on the other hand to be prepared for a freeze start at any time.
  • a previously common strategy for preparing for the freezing start provides for the longest possible time to be achieved in which an air / hydrogen front is prevented in the anode compartment when the fuel cell system is started. This always occurs when the hydrogen has diffused from the anode space 20 and air has penetrated. If fresh hydrogen is now replenished, this dreaded front occurs, which correspondingly damages the cathode and has an extremely disadvantageous and strong effect on the service life of the fuel cell 19.
  • the fuel cell system 2 in the embodiment variant shown here now has several options for preventing such an air / air start.
  • the first possibility is that the cathode space 21 can be evacuated accordingly. If there is no oxygen in this, the front cannot develop its damaging effect even if oxygen is present on the anode side and is displaced by the hydrogen flowing in at start-up.
  • This simple possibility can, for example, provide for the cathode to be kept permanently free of oxygen, which, given the tightness that usually occurs in the system, requires the cathode compartment 21 to be evacuated again, for example every 10 hours or the like. Since such a recurring evacuation is relatively risky for the membranes, since they can dry out, this procedure can be accompanied in particular with the moistening of the membranes described above if the temperatures are above freezing point and a safe and reliable start even with a certain residual moisture in the fuel cell 19 is possible.
  • a second possibility of avoiding an air / air start of the fuel cell 19 is that the air, which also entered the anode compartment 20 while the fuel cell system 2 was at a standstill, is sucked out of the anode compartment 20 again before the fuel cell 19 is started to evacuate it.
  • air is conveyed and flows via the cathode bypass 37 and the gas jet pump 38.
  • the purge valve 18 When the purge valve 18 is open, the air which has penetrated into the anode space 20 during the standstill can be sucked off. This makes it possible to at least significantly reduce the oxygen content in the volume of the anode space 20 and ultimately also of the anode circuit 28 before the start of the Fuel cell 19 is metered in hydrogen. This also enables a gentle start to be achieved and the service life of the fuel cell 19 to be extended.
  • the third option uses the generation of nitrogen or oxygen-depleted air, in particular air with an oxygen content of 0%, in order to achieve a very gentle start.
  • the circulation around the cathode space 21 is used for this. Hydrogen metered into the anode circuit 28 or residual hydrogen still present in it is sucked in via the gas jet pump 38 when the purge valve is open and thus enters the circuit together with the oxygen-containing air, which is caused by operation of the air compressor 1, which flows against the turbine side 13 of the freewheel 11 and so that the compressor side 10 moves, maintained.
  • the air then flows in a circle around the cathode compartment 21. It flows partly through the cathode compartment 21 and partly through the cathode bypass 37.
  • the fourth possibility to avoid an air / air start represents a combination of the second and the third possibility.
  • a hydrogen metering line 56 is required, via which hydrogen can be metered onto the cathode side. Similar to or as an alternative to the purge line 17, this hydrogen metering line 56 is connected to the gas jet pump 38 in the cathode bypass 37, as can be seen in the illustration of the figure. This makes it possible to supply hydrogen via the hydrogen metering line 56 to the To meter the cathode side of the fuel cell system 2 without this hydrogen having to flow through the anode space 20 beforehand.
  • the above-mentioned catalytic converter 55 which is connected downstream of the gas jet pump 38 in the circuit around the cathode chamber 21, can thus consume oxygen in the air. This is then autarkically recirculated in this circuit with the aid of the valve devices 35, 36, the valve 16 and the exhaust gas recirculation valve 24 and through the operation of the freewheel 11. This takes place until the oxygen content in the original air with the aid of the catalyst and the hydrogen entering the circuit via the hydrogen metering line 56 in the area of the mixing point in the gas jet pump 38 is less than 1 percent by volume, in particular to about 0 percent by volume is reduced. The then recirculated gas is thus virtually free of oxygen and essentially consists of nitrogen.
  • this gas is heated at the same time, which promotes the catalytic reaction in the catalytic converter 55 in order to efficiently convert oxygen and hydrogen.
  • a temperature range of approx. +60 to + 80 ° C is ideal for this. This allows the catalytic conversion to be regulated very well in order to avoid undesired nitrogen oxides within the closed volume. These nitrogen oxides as a by-product are undesirable because of the emissions of the same which occur later, but would not further impair the handling of the fuel cell 19, which is gentle on the service life.
  • the purge valve 18 can be opened, the freewheel 11 and thus ultimately the air compressor 1 can be switched off.
  • the cathode suction valve 40 and / or the valve devices 35, 36 are opened.
  • the nitrogen then flows back into the fuel cell 19 via the purge line and the cathode stub line and / or supply air line, so that it is filled with nitrogen. This enables an extremely gentle start of the fuel cell during next start process without the damaging mechanisms of the air / air start occurring.
  • a fifth possibility, in combination with the previously customary way of keeping the hydrogen in the system, can also be ideally used in the construction of the fuel cell system according to the invention.
  • the volumes of both the anode compartment 20 and the cathode compartment 21 are filled with hydrogen and kept under a slight overpressure in order to completely inert the volume through a hydrogen concentration of approximately 100 percent realize.
  • the residual hydrogen present in the cathode compartment 21 can now be removed again via the gas jet pump 38 and its operation through the supply air that has already been pumped but not flowing into the cathode compartment 21, in that the hydrogen is completely sucked out of the cathode compartment 21 before the cathode compartment 21 by opening the valve device 35 in the direction of the cathode chamber 21, oxygen or the air containing the oxygen is then acted upon in order to be able to start the fuel cell system 2 or its fuel cell 19.
  • the fuel cell 19 can be evacuated again using the gas jet pump 38 in the cathode bypass 37. With the purge valve 18 open, air can then be used with the air compressor switched off or oxygen-containing gas reach the area of the anode space 20.
  • the passive oxidation of carbon monoxide to carbon dioxide is conceivable. It becomes more efficient if the recirculation conveying device 31 is operated, for example by operating the air compressor 1 again with the purge valve 18 closed after air has flowed over into the anode circuit 28, in order to shape the recirculation conveying device 31 via the exhaust air turbine 32 in the exemplary embodiment shown here to drive the fan.
  • the refresh of the catalytic converter is then completed after a short time, for example on the order of less than a minute.
  • the oxygen-containing gas can then be sucked out of the anode circuit again by opening the purge valve 18 again and the system can be filled with nitrogen in the manner described above, for example, in order to prepare it for the next start.
  • Air compressor 28 Anode circuit, fuel cell system 29 Recirculation line, air delivery device 30 Water separator, electric motor 31 Recirculation delivery device, shaft 32 Exhaust air turbine, second compressor wheel 33 Shaft, first compressor wheel 34 Liquid water system, suction path 35 Valve device, register line 36 Valve device, compressor side 37 Cathode bypass, Free-running turbocharger, water separator, cathode line, 41, Turbocharger, cathode tank line, 42, Turbocharger, cathode tank line, 40, Turbocharger, gas jet pump, shaft 43 Arrow blow-off line 44 thermal insulation purge valve 45 water pump fuel cell stack 46 branch line anode compartment 47 humidifier cathode compartment 48 humidifier supply air line 49 branch line exhaust air line 50 pressure water distributor exhaust gas recirculation valve 51 branch exhaust gas recirculation line 52 branch line fuel 53 hydrodynamic bearing supply device 54 hydrodynamic bearing pressure control and 55 catalyst dos i device 56 hydrogen metering line

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  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
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Abstract

L'invention concerne un système de pile à combustible (2) comprenant au moins un empilement de cellules (19) qui délimite une chambre anodique (20) et une chambre cathodique (21), au moins un dispositif d'acheminement d'air (3) pour alimenter la chambre cathodique (21) en air par l'intermédiaire d'une conduite d'amenée d'air (22), une conduite d'évacuation d'air (23) partant de la chambre cathodique (21), au moins un dispositif d'alimentation en combustible (26) pour alimenter la chambre anodique (20) en combustible, au moins un circuit anodique (28) pour la recirculation du combustible non consommé autour de la chambre anodique (20), ainsi qu'une dérivation cathodique (37). Le système de pile à combustible selon l'invention est caractérisé en ce que la conduite de dérivation cathodique (37) part de la conduite d'amenée d'air (22) en amont ou au niveau d'un dispositif de soupape (35) dans ladite conduite d'amenée d'air (22) et débouche dans la conduite d'évacuation d'air (23) en aval ou au niveau d'un autre dispositif de soupape (36) dans ladite conduite d'évacuation d'air (23). Une pompe à jet de gaz (38) qui peut être entraînée par l'air s'écoulant autour de la chambre cathodique (21) est placée dans la dérivation cathodique (37), cette pompe étant reliée de manière commutable côté aspiration à la chambre anodique (20) et/ou à la chambre cathodique (21).
EP21726616.2A 2020-05-15 2021-05-12 Système de pile à combustible Pending EP4150689A2 (fr)

Applications Claiming Priority (2)

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DE102020206156.4A DE102020206156A1 (de) 2020-05-15 2020-05-15 Brennstoffzellensystem
PCT/EP2021/062573 WO2021228915A2 (fr) 2020-05-15 2021-05-12 Système de pile à combustible

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US (1) US20230197988A1 (fr)
EP (1) EP4150689A2 (fr)
JP (1) JP7474353B2 (fr)
KR (1) KR20230013048A (fr)
CN (1) CN115552671A (fr)
DE (1) DE102020206156A1 (fr)
WO (1) WO2021228915A2 (fr)

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Publication number Priority date Publication date Assignee Title
DE102020007745A1 (de) 2020-12-18 2022-06-23 Cellcentric Gmbh & Co. Kg Vorrichtung zur Luftversorgung einer Brennstoffzelle
DE102021206676A1 (de) 2021-06-28 2022-12-29 Cellcentric Gmbh & Co. Kg Verfahren zur Reinigung eines Rezirkulationskreislaufs
DE102022203514A1 (de) * 2022-04-07 2023-10-12 Robert Bosch Gesellschaft mit beschränkter Haftung Verfahren zum Betreiben eines Brennstoffzellensystems
DE102022204143A1 (de) 2022-04-28 2023-11-02 Robert Bosch Gesellschaft mit beschränkter Haftung Brennstoffzellensystem und Trocknungsverfahren zum Trocknen von Brennstoffzellen eines Brennstoffzellensystems

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Publication number Priority date Publication date Assignee Title
US6432568B1 (en) * 2000-08-03 2002-08-13 General Motors Corporation Water management system for electrochemical engine
DE102007037096A1 (de) * 2007-08-07 2009-02-12 Daimler Ag Verfahren und Vorrichtung zum Betreiben eines Brennstoffzellensystems mit einem in einen Brennstoffkreislauf des Brennstoffzellensystems angeordneten Rezirkulationsgebläse
US8057942B2 (en) 2007-10-18 2011-11-15 GM Global Technology Operations LLC Assisted stack anode purge at start-up of fuel cell system
DE102009043569A1 (de) 2009-09-30 2011-04-07 Daimler Ag Verfahren zum Betreiben eines Brennstoffzellensystems
JP5601362B2 (ja) * 2012-10-16 2014-10-08 トヨタ自動車株式会社 内燃機関
DE102014207450A1 (de) * 2014-04-17 2015-10-22 Bayerische Motoren Werke Aktiengesellschaft Verfahren zum Spülen einer Brennstoffzelle sowie Vorrichtung zur Durchführung des Verfahrens
DE102014221321A1 (de) 2014-10-21 2016-04-21 Volkswagen Ag Brennstoffzellensystem sowie Verfahren zum Abschalten eines Brennstoffzellenstapels
DE102017204110A1 (de) * 2017-03-13 2018-09-13 Bayerische Motoren Werke Aktiengesellschaft Verfahren zum Erfassen von Leckage-Brennstoff sowie Brennstoffzellensystem
DE102017220855A1 (de) * 2017-11-22 2019-05-23 Robert Bosch Gmbh Turbokompressor, insbesondere für ein Brennstoffzellensystem
DE102018202906A1 (de) * 2018-02-27 2019-08-29 Robert Bosch Gmbh Brennstoffzellensystem

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WO2021228915A8 (fr) 2022-02-03
JP7474353B2 (ja) 2024-04-24
JP2023524851A (ja) 2023-06-13
WO2021228915A3 (fr) 2021-12-23
DE102020206156A1 (de) 2021-11-18
WO2021228915A2 (fr) 2021-11-18
CN115552671A (zh) 2022-12-30
US20230197988A1 (en) 2023-06-22
KR20230013048A (ko) 2023-01-26

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