EP4324957A1 - Procédé et installation de fabrication d'un produit contenant de l'hydrogène - Google Patents

Procédé et installation de fabrication d'un produit contenant de l'hydrogène Download PDF

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Publication number
EP4324957A1
EP4324957A1 EP22020401.0A EP22020401A EP4324957A1 EP 4324957 A1 EP4324957 A1 EP 4324957A1 EP 22020401 A EP22020401 A EP 22020401A EP 4324957 A1 EP4324957 A1 EP 4324957A1
Authority
EP
European Patent Office
Prior art keywords
cathode
feed gas
gas
hydrogen
steam
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
EP22020401.0A
Other languages
German (de)
English (en)
Inventor
Harald Klein
Johanna HEMAUER
Steffen Fahr
Andreas Peschel
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.)
Linde GmbH
Technische Universitaet Muenchen
Original Assignee
Linde GmbH
Technische Universitaet Muenchen
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 Linde GmbH, Technische Universitaet Muenchen filed Critical Linde GmbH
Priority to EP22020401.0A priority Critical patent/EP4324957A1/fr
Publication of EP4324957A1 publication Critical patent/EP4324957A1/fr
Pending legal-status Critical Current

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    • 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
    • C25B1/042—Hydrogen or oxygen by electrolysis of water by electrolysis of steam
    • 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
    • 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
    • C25B9/05—Pressure cells
    • 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
    • C25B9/70—Assemblies comprising two or more cells

Definitions

  • the present invention relates to a method and a system for producing a hydrogen-containing product using a solid oxide electrolysis cell.
  • SOEC solid oxide electrolysis cells
  • a water molecule reacts with two electrons at the cathode to form a hydrogen molecule and an oxygen ion.
  • an oxygen ion reacts to form (mathematically) half an oxygen molecule and two electrons.
  • the oxygen ions are the charge carriers.
  • High-temperature electrolysis which is carried out using one or more solid oxide electrolysis cells, can also be used to electrochemically produce carbon monoxide from carbon dioxide. This creates oxygen on the anode side and carbon monoxide on the cathode side.
  • WO 2014/154253 A1 the WO 2013/131778 A2 , the WO 2015/014527 A1 and the EP 2 940 773 A1 referred.
  • Co-electrolysis of water and carbon dioxide in appropriate facilities is also possible.
  • hydrogen and carbon monoxide are formed at the cathode.
  • Co-electrolysis can also be used at any time within the scope of the present invention.
  • a product containing hydrogen and carbon monoxide i.e. so-called synthesis gas is then obtained.
  • the present invention aims to improve the production of hydrogen or hydrogen-containing products (a hydrogen-containing product can be a mixture of hydrogen and other components or pure hydrogen) using solid oxide electrolysis cells.
  • the present invention proposes a method and a system for obtaining a hydrogen-containing product using a solid oxide electrolysis cell with the features of the independent patent claims. Refinements are the subject of the dependent claims and the description.
  • embodiments of the present invention are typically implemented with several such cells, whereby corresponding cells can in particular be part of a cell stack of a known type, in in which such cells are present in large numbers.
  • multiple stacks can be used in parallel.
  • a plurality of arrangements consisting of anode, electrolyte and cathode are provided, each of which is separated from one another by separating plates with channels.
  • the channels are typically formed parallel to each other in the top and bottom of the separating plates.
  • the channels on the top and bottom are arranged at an angle of, for example, 90° to one another and enable the respective gases or gas mixtures to be fed in or removed from the anode and cathode sides. They are connected to feed or collecting lines that supply the entire stack.
  • an “anode side” or “cathode side” of a high-temperature or solid oxide electrolysis cell these terms can also refer to the cathode sides or anode sides of the cells of corresponding cell stacks in total.
  • a gas mixture supplied as a whole to this cathode side(s) is also referred to below as “cathode feed gas”, and a gas removed as a whole from the cathode side(s) is also referred to below as “cathode extraction gas”.
  • cathode feed gas a gas removed as a whole from the cathode side(s)
  • cathode extraction gas The same applies to the anode side, i.e. also for “anode feed gas” or “anode extraction gas”.
  • high-temperature or solid oxide electrolysis cells of the type explained at the beginning can be used to convert water into hydrogen using electrical energy. Since high-temperature or solid oxide electrolysis cells operate at temperatures of 550 or 600 to 950 °C, the water in the cathode feed gas must be provided as steam.
  • thermoneutral voltage indicates the potential in which the heat generated by the current flow is equal to the heat consumption during the cell reaction.
  • the thermal energy balance is zero at thermoneutral voltage.
  • a hot mixture of hydrogen and uncondensed steam on the one hand or oxygen-rich air on the other always leaves the cell or stack on the cathode or anode side (and thus as cathode or anode extraction gas in the language used here).
  • Some of the steam required for the high-temperature or solid oxide electrolytic cells can be generated by heat integration with the hot cathode and anode extraction gas. Additional steam can either be imported or generated internally, which uses energy.
  • hydrogen can be partially returned to the cathode side after cooling, separation of water and compression in the cathode feed gas. Details are related below Figure 1 explained.
  • Typical values for the molar proportion of hydrogen in the cathode feed gas are 10% or more, so that a high steam conversion is particularly important for an efficient process in high-temperature or solid oxide electrolysis cells.
  • the steam conversion depends on many parameters, e.g. on the temperature, the current density and the flow rate. High steam conversion is possible at lower flow rates; consequently, at higher flow rates, steam conversion decreases.
  • the current density can be increased (at high flow rates) so that the overall performance of the cell in terms of hydrogen production per volume at thermoneutral voltage increases. This is particularly advantageous in terms of reducing investment costs.
  • the cathode extraction gas is cooled so that the uncondensed residual vapor in it can be condensed and separated from the hydrogen.
  • “dry” hydrogen which is also cooled due to condensation, can be obtained.
  • compression typically occurs.
  • the required hydrogen is provided by recycling a portion of the hot cathode extraction gas from uncondensed steam and hydrogen before a corresponding condensation. In this way, in embodiments of the invention, part of the unconverted steam can be recovered or further used.
  • a process for producing a hydrogen-containing product as mentioned for example pure or essentially pure hydrogen, but also, for example, a synthesis gas in the case of co-electrolysis, is proposed.
  • one or more solid oxide electrolysis cells in one or more stacks, as explained above are used, to which a cathode feed gas containing hydrogen and uncondensed steam is supplied on the cathode side and a cathode feed gas containing more hydrogen and less uncondensed steam than the cathode feed gas containing cathode extraction gas is removed.
  • the respective contents or ratios to each other depend on the steam conversion.
  • the cathode feed gas can, for example, contain 5 to 20%, in particular 10 to 15%, hydrogen and the rest steam or a mixture of steam, carbon dioxide and carbon monoxide.
  • the hydrogen content in the cathode extraction gas, or in the case of co-electrolysis a total content of hydrogen and carbon monoxide can be, for example, 30 to 80%, in particular 50 to 70%.
  • the cathode feed gas is formed using a subset of the cathode extraction gas containing uncondensed steam and hydrogen and process steam. As mentioned, no steam condensation occurs, but rather a portion of the residual steam is uncondensed and returned, especially in the hot state.
  • the subset of the cathode extraction gas used to form the cathode feed gas or a part thereof and a further subset of the cathode extraction gas that is not used in the formation of the cathode feed gas and contains uncondensed steam and hydrogen Cathode extraction gas or a part thereof is subjected to a common cooling against the cathode feed gas or a part thereof.
  • a known feed-effluent heat exchanger can be used for this cooling.
  • the advantage of this configuration is, in particular, that high-temperature heat is recovered and the power requirement in the high-temperature electrolysis and in the cathode preheater can be reduced.
  • lower demands may be placed on the compressor or ejector than in cases in which the stream is combined with hot process gas before cooling and compressed or fed into the ejector, or compression before the merger is carried out.
  • Feed-effluent heat exchangers are often used in reactors, for example to carry out exothermic adiabatic high-temperature reactions, especially in tubular reactor systems, in order to recover energy.
  • a hot medium flowing from the reactor is used in an appropriate feed-effluent heat exchanger to provide all or part of the energy required to preheat the reactor feed to the optimal reactor inlet temperature.
  • Different concepts can be used for temperature regulation, which can also be used in embodiments of the present invention.
  • a bypass can be routed around the feed-effluent heat exchanger, but additional, adjustable heating or cooling devices can also be used, for example between the feed-effluent heat exchanger and the reactor.
  • a number of control structures are known for regulating the reactor inlet temperature, which can also be used in embodiments of the invention.
  • Appropriate control structures are also crucial for dynamic performance, as such systems can be unstable due to the positive feedback of energy from the reactor back into the preheating system.
  • a corresponding control structure can influence a bypass around the feed-effluent heat exchanger, if present, or a cooling or heating output of the heating or cooling device, if present.
  • This embodiment can further include that the subset of the cathode extraction gas used to form the cathode feed gas or a part thereof is combined with the process steam or a part thereof to form a collecting stream after the joint cooling.
  • the collecting stream is subjected to compression in a compressor after the combination, but it can also be that the collecting stream is formed by feeding it into an ejector.
  • a combination downstream of this is also possible, i.e. the subset of the cathode extraction gas used to form the cathode feed gas can be subjected to compression in a compressor or fed into an ejector before the combination.
  • combinations of compressors and ejectors can be used to achieve the required pressure.
  • a pressurized medium in this case the process steam or part thereof, is typically guided through a Venturi nozzle.
  • the pressurized medium is further pressurized and accelerated in the Venturi nozzle.
  • the accelerated, pressurized medium relaxes and a negative pressure is created.
  • a further medium in the present case the recirculated portion of the cathode extraction gas or a portion thereof
  • the subset of the cathode extraction gas used to form the cathode feed gas or a portion thereof and the heated process steam or a portion thereof can be subjected to combination to form a collection stream in this embodiment.
  • the collecting stream is subjected to compression in a compressor after the combination, but it can also be that the collecting stream is formed by feeding it into an ejector.
  • the subset of the cathode extraction gas used to form the cathode feed gas is subjected to compression in a compressor or fed into an ejector before combining.
  • combinations of compressors and ejectors can be used to achieve the required pressure.
  • the further subset of the cathode extraction gas not used to form the cathode feed gas or a portion thereof can be subjected to water separation in embodiments of the invention in order to form the hydrogen-containing product in this way.
  • this can be done as in known methods, so that no further explanations are required.
  • the cathode feed gas, the cathode extraction gas, the subset of the cathode extract gas used to form the cathode feed gas and the further subset of the cathode feed gas not used to form the cathode feed gas can also include carbon dioxide, which is converted into carbon monoxide in the one or more solid oxide electrolysis cells, and that transferred in a known manner into the corresponding material streams.
  • the carbon dioxide is only partially converted, so that the cathode extraction gas contains carbon monoxide and carbon dioxide.
  • the hydrogen-containing product can also be synthesis gas and some of the carbon monoxide in the cathode extraction gas is also recycled into the cathode feed gas.
  • the invention can therefore also be implemented in connection with a corresponding co-electrolysis.
  • freshly used carbon dioxide is supplied via the process steam.
  • process steam process steam containing carbon dioxide can also be meant.
  • the one or more solid oxide electrolysis cells or one or more stacks in a corresponding system 40 to 80% or 40 to 60% of the amount of steam supplied in the cathode feed gas can be converted.
  • the advantages of the present invention include higher efficiency due to energy savings through improved heat and material integration, these advantages being particularly important when the steam conversion is low, around 50%.
  • different configurations and designs were examined with regard to their impact on the system efficiency (based on the upper heating value).
  • a conventional recirculation of dry hydrogen with a steam conversion of 50% resulted in a system efficiency of 0.769, which increased to 0.798 in an embodiment of the invention with a compressor and recirculation of a subset of the cathode extraction gas containing uncondensed steam and hydrogen and a steam conversion of 50%.
  • a slightly lower system efficiency of 0.793 resulted under the same conditions but using an ejector.
  • the one or more solid oxide electrolysis cells can be operated at a pressure level of 1 to 30 bar, in particular 1 to 7 bar absolute pressure.
  • the lower limit of the operating pressure range is slightly above atmospheric pressure, for example at 10, 50, 100 or 500 mbar overpressure.
  • a system for producing a hydrogen-containing product is also the subject of the present invention, wherein the system has one or more solid oxide electrolysis cells, the system being set up to supply a cathode feed gas containing hydrogen and uncondensed steam to the one or more solid oxide electrolysis cells on the cathode side and extracting a cathode extraction gas containing more hydrogen and less uncondensed steam than the cathode feed gas, and wherein the system is adapted to form the cathode feed gas using a subset of the cathode extraction gas and process steam containing uncondensed steam and hydrogen.
  • Different embodiments of the invention may include, have, consist of, or consist essentially of other useful combinations of the described elements, components, features, parts, steps, means, etc., even if such combinations are not specifically described herein.
  • the disclosure may include other inventions that are not currently claimed but that may be claimed in the future, particularly if included within the scope of the independent claims.
  • the method is used to produce a hydrogen-containing product 110, using one or more solid oxide electrolysis cells 10, in particular in a corresponding stack.
  • An anode feed gas 201 for example air, is supplied to an anode side 11, and a corresponding anode extraction gas 202 is withdrawn from the anode side 11.
  • a cathode feed gas 101 containing hydrogen and uncondensed steam is supplied and a cathode extraction gas 102 containing more hydrogen and less uncondensed steam than the cathode feed gas 101 is removed.
  • this is Cathode extraction gas 102 is subjected to a heat exchange 20 with the cathode feed gas 101 in a feed-effluent heat exchanger.
  • steam can be generated in a heat integration 60. Any other options for heat integration 60 can be implemented. In this way, steam can be generated and water can also be preheated in another heat exchanger, which is then evaporated in a corresponding evaporator.
  • the heat integration 60 takes place before a condensation of water 109 is carried out in a stepwise compression and cooling 50, so that a hydrogen stream or a gas mixture containing hydrogen remains as product 110.
  • a partial stream 108 of the dry and compressed hydrogen is mixed with process steam 104 to form a collection stream 105, then subjected to the heat exchange 20 and a further heat exchange 70, and fed back to the cathode side as the cathode feed gas 101 mentioned.
  • the cathode feed gas 101 is formed here using a subset 103 of the cathode extraction gas 102 and the process steam 104 containing uncondensed steam and hydrogen.
  • the subset 103 of the cathode extraction gas 102 used to form the cathode feed gas 101 and a further subset 106 of the cathode extraction gas that is not used in the formation of the cathode feed gas 101 and contains uncondensed steam and hydrogen are subjected to a common cooling 20 against the cathode feed gas 101. Furthermore, the subset 103 of the cathode extraction gas 102 used to form the cathode feed gas 101 and the process steam 104 upstream of the common cooling 20 are subjected to a combination to form the collecting stream 105.
  • the collection stream 105 is subjected to compression in a compressor 30 after combining, whereas the Unification in the in Figure 3 illustrated embodiment of the method 200 by feeding into an ejector 40.
  • Illustrated embodiments or methods 300 and 400 include that a further subset of the cathode extraction gas 106, which is not used to form the cathode feed gas 101 and contains uncondensed steam and hydrogen, but not the subset 103 of the cathode extraction gas 102 used to form the cathode feed gas 101, against the process steam ( optionally with components of carbon dioxide) 104 is cooled, whereby heated process steam 107 is formed.
  • the subset 103 of the cathode extraction gas 102 used to form the cathode feed gas 101 and the heated process steam 107 are subjected to a combination to form the collection stream 105.
  • the collection stream 105 is subjected to compression in a compressor 30 after the combination, whereas the combination in the in Figure 5 illustrated embodiment of the method 400 takes place by feeding into an ejector 40.
  • the heat integration 60 or a corresponding steam generator is illustrated downstream of the heat exchanger 20, i.e. downstream of a feed-effluent heat exchanger, in certain cases, Particularly in the case of co-electrolysis with synthesis gas in the cathode extraction gas, it may be advantageous to arrange a corresponding steam generator upstream of the feed-effluent heat exchanger. This can in particular ensure rapid cooling and prevent further reactions.
  • the return quantity i.e. the partial quantity 103 of the cathode extraction gas 102 containing uncondensed steam and hydrogen, can be withdrawn upstream of a corresponding steam generator or between the steam generator and the feed-effluent heat exchanger.

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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)
EP22020401.0A 2022-08-19 2022-08-19 Procédé et installation de fabrication d'un produit contenant de l'hydrogène Pending EP4324957A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP22020401.0A EP4324957A1 (fr) 2022-08-19 2022-08-19 Procédé et installation de fabrication d'un produit contenant de l'hydrogène

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EP22020401.0A EP4324957A1 (fr) 2022-08-19 2022-08-19 Procédé et installation de fabrication d'un produit contenant de l'hydrogène

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EP4324957A1 true EP4324957A1 (fr) 2024-02-21

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Citations (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2013131778A2 (fr) 2012-03-05 2013-09-12 Haldor Topsøe A/S Appareil de production de monoxyde de carbone de haute pureté
WO2014154253A1 (fr) 2013-03-26 2014-10-02 Haldor Topsøe A/S Procédé de production de co à partir de co2 dans une cellule d'électrolyse à oxyde solide
WO2015014527A1 (fr) 2013-07-30 2015-02-05 Haldor Topsøe A/S Processus de production de co à haute pureté par purification par membrane du co produit par une pile à électrolyse à oxyde solide (soec)
EP2940773A1 (fr) 2014-04-29 2015-11-04 Haldor Topsøe A/S Éjecteur pour système d'empilement de cellule d'électrolyse d'oxyde solide
WO2016161999A1 (fr) * 2015-04-08 2016-10-13 Sunfire Gmbh Procédé de gestion de chaleur d'une électrolyse à vapeur d'eau à haute température [soec], cellule de combustible à oxyde solide [sofc] et/ou cellule de combustible à haute température réversible [rsoc] ainsi qu'un système d'électrolyse à vapeur d'eau à haute température [soec], de cellule de combustible à oxyde solide [sofc] et/ou de cellule de combustible à haute température réversible
US20170175277A1 (en) * 2014-06-06 2017-06-22 Sunfire Gmbh Electrolysis method and electrolyis system comprising recirculating flushing media
US20200095124A1 (en) * 2017-06-12 2020-03-26 Sunfire Gmbh Synthesis gas production from co2 and h2o in a co-electrolysis
EP3766831A1 (fr) 2019-07-18 2021-01-20 Linde GmbH Procédé de fonctionnement d'un four chauffé et agencement comprenant un tel four
EP3869599A1 (fr) * 2019-03-25 2021-08-25 Korea Institute of Machinery & Materials Système réversible d'électrolyse de l'eau et son procédé de fonctionnement

Patent Citations (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2013131778A2 (fr) 2012-03-05 2013-09-12 Haldor Topsøe A/S Appareil de production de monoxyde de carbone de haute pureté
WO2014154253A1 (fr) 2013-03-26 2014-10-02 Haldor Topsøe A/S Procédé de production de co à partir de co2 dans une cellule d'électrolyse à oxyde solide
WO2015014527A1 (fr) 2013-07-30 2015-02-05 Haldor Topsøe A/S Processus de production de co à haute pureté par purification par membrane du co produit par une pile à électrolyse à oxyde solide (soec)
EP2940773A1 (fr) 2014-04-29 2015-11-04 Haldor Topsøe A/S Éjecteur pour système d'empilement de cellule d'électrolyse d'oxyde solide
US20170175277A1 (en) * 2014-06-06 2017-06-22 Sunfire Gmbh Electrolysis method and electrolyis system comprising recirculating flushing media
WO2016161999A1 (fr) * 2015-04-08 2016-10-13 Sunfire Gmbh Procédé de gestion de chaleur d'une électrolyse à vapeur d'eau à haute température [soec], cellule de combustible à oxyde solide [sofc] et/ou cellule de combustible à haute température réversible [rsoc] ainsi qu'un système d'électrolyse à vapeur d'eau à haute température [soec], de cellule de combustible à oxyde solide [sofc] et/ou de cellule de combustible à haute température réversible
US20200095124A1 (en) * 2017-06-12 2020-03-26 Sunfire Gmbh Synthesis gas production from co2 and h2o in a co-electrolysis
EP3869599A1 (fr) * 2019-03-25 2021-08-25 Korea Institute of Machinery & Materials Système réversible d'électrolyse de l'eau et son procédé de fonctionnement
EP3766831A1 (fr) 2019-07-18 2021-01-20 Linde GmbH Procédé de fonctionnement d'un four chauffé et agencement comprenant un tel four

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