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WO2022022849A1 - Maintien de pression dans un système d'électrolyse - Google Patents

Maintien de pression dans un système d'électrolyse Download PDF

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Publication number
WO2022022849A1
WO2022022849A1 PCT/EP2021/025225 EP2021025225W WO2022022849A1 WO 2022022849 A1 WO2022022849 A1 WO 2022022849A1 EP 2021025225 W EP2021025225 W EP 2021025225W WO 2022022849 A1 WO2022022849 A1 WO 2022022849A1
Authority
WO
WIPO (PCT)
Prior art keywords
gas
pressure
space
carbon dioxide
anode
Prior art date
Application number
PCT/EP2021/025225
Other languages
German (de)
English (en)
Inventor
Andreas Peschel
Benjamin HENTSCHEL
Original Assignee
Linde Gmbh
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 filed Critical Linde Gmbh
Publication of WO2022022849A1 publication Critical patent/WO2022022849A1/fr

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Classifications

    • 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
    • C25B1/23—Carbon monoxide or syngas
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B15/00—Operating or servicing cells
    • C25B15/08—Supplying or removing reactants or electrolytes; Regeneration of electrolytes
    • C25B15/087—Recycling of electrolyte to electrochemical cell
    • 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
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
    • C25B9/21—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms two or more diaphragms
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B9/00—Cells or assemblies of cells; Constructional parts of cells; Assemblies of constructional parts, e.g. electrode-diaphragm assemblies; Process-related cell features
    • C25B9/17—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof
    • C25B9/19—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms
    • C25B9/23—Cells comprising dimensionally-stable non-movable electrodes; Assemblies of constructional parts thereof with diaphragms comprising ion-exchange membranes in or on which electrode material is embedded

Definitions

  • the invention relates to a method and a plant for producing carbon monoxide from carbon dioxide according to the preambles of the independent patent claims.
  • Carbon monoxide an important raw material in the chemical industry, can in principle be produced using various processes. For example, steam reforming or dry reforming of natural gas or other high-carbon fossil feedstocks is possible.
  • oxygen and/or hydrogen can also be formed in addition to carbon monoxide.
  • protons are selectively transferred from the anode to the cathode side via a membrane. Then they compete at the cathode Hydrogen and the carbon monoxide formation reaction, resulting in a product gas with different hydrogen/carbon monoxide ratio. Almost pure carbon monoxide can also be generated in the process.
  • a particularly interesting application of carbon dioxide electrolysis is the on-site production of carbon monoxide, with membrane-based carbon dioxide separation being very advantageous for small to medium-sized production quantities due to the moderate investment costs.
  • the flexibility of the plant often also plays a decisive role, either due to a changing carbon monoxide requirement over time, for example if carbon monoxide is required as a starting material in batch processes, or in order to be able to participate in the fluctuating energy market in order to be able to to reduce production costs.
  • Low-temperature electrolysers in particular are extremely well suited for flexible operation due to their fast dynamics.
  • a method for the electrolytic production of carbon monoxide from carbon dioxide comprises the use of an electrolysis device which has an anode compartment, a cathode compartment and a gas compartment, the anode compartment being separated from the cathode compartment by an ion-conducting membrane and the cathode compartment being separated from the gas compartment by a gas diffusion electrode.
  • the cathode space is located between the anode space and the gas space
  • the ion-conducting membrane is located between the anode space and the cathode space
  • the gas diffusion electrode is located between the cathode space and the gas space.
  • the anode compartment is operated at an anode compartment pressure, the cathode compartment at a cathode compartment pressure and the gas compartment at a gas compartment pressure, a liquid anolyte being fed to the anode compartment, a liquid catholyte to the cathode compartment and gaseous carbon dioxide to the gas compartment.
  • gases particularly carbon dioxide
  • gases in the supercritical state are considered “gaseous” for the purposes of this disclosure. So if a "gaseous" substance is mentioned, the same substance in the supercritical state should also be included.
  • a first portion of the carbon dioxide supplied to the gas space is converted to carbon monoxide at the gas diffusion electrode, while a second portion of the carbon dioxide passes through the gas diffusion electrode into the catholyte. (Another part can pass through the gas space unreacted.)
  • the carbon monoxide formed in this way and present in the gas space is from the Gas space discharged in the form of a raw gas.
  • the second part of the carbon dioxide is at least partially discharged with the catholyte from the cathode space, at least partially removed from the catholyte, and returned to the gas space without mechanical compression.
  • the gas space pressure is kept at a pressure which, according to the invention, is 100 kPa below and 10 kPa above the cathode space pressure.
  • the gas space pressure is 100 kPa below to 5 kPa below the cathode space pressure, in particular in a range from 100 kPa to 10 kPa, from 100 kPa to 20 kPa, from 100 kPa to 30 kPa, from 100 kPa to 40 kPa , specifically from 100 kPa to 50 kPa below the cathode compartment pressure.
  • a transfer of carbon dioxide can be prevented in a particularly reliable manner by a corresponding pressure drop across the gas diffusion electrode if a sufficiently pressure-resistant gas diffusion electrode is used in the method.
  • the pressure level of the gas space is nevertheless high enough to prevent the catholyte from escaping into the gas space.
  • the pressures in the cathode space and gas space can also be essentially the same, i.e. the gas space pressure is then in particular 10 kPa below to 10 kPa above the cathode space pressure.
  • the gas space pressure is then in particular 10 kPa below to 10 kPa above the cathode space pressure.
  • the use of the present invention results in a simpler configuration of the electrolysis process, which also makes use in the application scenarios explained at the outset advantageous.
  • the anode compartment pressure is between 10 kPa below and 10 kPa above the cathode compartment pressure. The three pressures are thus very similar or substantially equal to each other. As a result, the membrane between the anode and the cathode space is relieved.
  • the anode compartment pressure can also be significantly below the cathode compartment pressure, in particular if the electrolysis is carried out using a high-pressure electrolyzer. It is important to ensure that the membrane, which separates the anode from the cathode space, is not damaged by the large pressure difference.
  • This can be implemented, for example, by using a PEM, as is described elsewhere in this application, optionally in conjunction with a corresponding mechanical support element.
  • the anode compartment pressure can therefore be up to 7 MPa below the pressure level at which the anode compartment and gas compartment are operated. This offers the advantage that the oxygen that is formed on the anode side occurs at a low pressure level, which is desirable from a safety standpoint and considerably simplifies the selection of materials for components on the anode side.
  • oxygen that is produced during the electrolysis in gaseous form or dissolved in the anolyte in the anode compartment is at least partially discharged with the anolyte from the anode compartment, removed from the anolyte and discharged from the process via a control valve.
  • input variables that characterize, for example, the anode chamber pressure and the cathode chamber pressure and/or the gas chamber pressure can be detected and the anode chamber pressure can be changed by setting the control valve.
  • This can be done in a controlled, regulated manner or in a manner that can be set manually by an operator, the detected input variables preferably being taken into account.
  • an optimal position of the control valve can be determined by comparing the pressures characterized by the input variables. This enables precise control of the process so that overall efficiency can be maximized.
  • an automated procedure is possible because the control or regulation can be taken over by a computing unit that is programmed accordingly.
  • a further possibility is the design of the control valve for a predefinable pressure loss, which results in self-regulation via the flow rate through the valve. This alternative is particularly robust and low-maintenance.
  • the carbon dioxide supplied to the gas space can contain other gas components, for example inert gases such as nitrogen and/or argon or electrolyzable gases such as steam. This allows the composition of the process product to be adjusted and/or the pressure adjustment to be facilitated, particularly in a case in which carbon dioxide is available in fluctuating amounts.
  • inert gases such as nitrogen and/or argon or electrolyzable gases such as steam.
  • the fresh feed can be fed into the plant at a suitable point.
  • it can be fed directly into the gas space, but the fresh feed can also be combined with the carbon dioxide recycled from the catholyte upstream of the gas space or into a gas separator provided for removing the carbon dioxide from the catholyte.
  • a gas separator provided for removing the carbon dioxide from the catholyte.
  • it is particularly important to ensure that the fresh charge is introduced above the liquid level in order to avoid additional release of carbon dioxide from the fresh charge in the catholyte.
  • This arrangement is advantageous, for example, when the pressure of the carbon dioxide separated from the catholyte is too low, ie the gas space is operated in particular at a pressure level which is below the pressure level of the catholyte space.
  • Valves which can be provided for control between the gas separator and the electrolysis, can advantageously reduce the effect of pressure fluctuations in the fresh charge on the gas space and thus on the gas diffusion electrode.
  • hydrogen can also be formed, which is preferably discharged from the gas space together with the carbon monoxide.
  • a product of Process with a composition adapted to different requirements are produced specifically.
  • the gas space pressure is particularly preferably set to a pressure level in a range between 110 kPa and 7 MPa.
  • the method can be flexibly adapted to changes in requirements, so that, for example, the product of the method occurs at a pressure level that corresponds to an input pressure level of a further processing process.
  • a pressure level is to be understood as meaning a pressure within a pressure range whose limits differ by at most 1%, 2%, 5%, 10% or 20% from an average value of the respective pressure range.
  • a pressure level of 1 MPa for example, is accordingly in a range from at least 800 kPa to a maximum of 1.2 MPa.
  • the anolyte preferably contains at least water and/or consists of it to a large majority. This represents a particularly inexpensive variant that is easy to obtain.
  • the anolyte is provided in the form of an (ion-conducting) electrode, insofar as separation from the catholyte circuit is ensured.
  • the catholyte preferably contains water and/or an aqueous base, for example an aqueous solution of lithium carbonate, sodium carbonate, potassium carbonate, strontium carbonate, lithium hydroxide, sodium hydroxide, potassium hydroxide, strontium hydroxide and/or ammonia.
  • an aqueous solution of lithium carbonate, sodium carbonate, potassium carbonate, strontium carbonate, lithium hydroxide, sodium hydroxide, potassium hydroxide, strontium hydroxide and/or ammonia aqueous solution of lithium carbonate, sodium carbonate, potassium carbonate, strontium carbonate, lithium hydroxide, sodium hydroxide, potassium hydroxide, strontium hydroxide and/or ammonia.
  • electrolysis is preferably carried out using a low-temperature co-electrolysis, a low-temperature electrolysis, a low-pressure electrolysis and/or a high-pressure electrolysis, since this in turn allows the process to be adapted to the required product quality and/or the starting materials available.
  • a further aspect of the invention relates to a system, with regard to the features of which reference is expressly made to the above statements relating to the method according to the invention.
  • the system has a correspondingly pressure-stable gas diffusion electrode when working with a pressure gradient between the cathode chamber pressure and the gas chamber pressure.
  • the gas diffusion electrode is designed in such a way that the phase boundary between the gaseous carbon dioxide and the generally liquid catholyte is located within the electrode.
  • a pore size distribution and/or a hydrophobicity of the gas diffusion electrode can be specifically set in such a way that this is guaranteed for the planned pressure difference between the gas space and the cathode space.
  • FIG. 1 schematically shows a preferred embodiment of an electrolysis device according to the invention.
  • the electrolysis device 100 shown schematically in Figure 1 comprises an electrolysis cell which is divided into three spaces: an anode space 10, a cathode space 20 and a gas space 30.
  • the anode space 10 is separated from the cathode space 20 by an ion-conducting membrane M, the cathode space from the gas space delimited by a gas diffusion electrode K.
  • the membrane M can be designed, for example, as a proton exchange membrane (PEM), cation exchange membrane, anion exchange membrane, glass frit, ceramic, metal or polymer membrane or another suitable selectively or nonselectively permeable membrane.
  • PEM proton exchange membrane
  • the gas diffusion electrode K can be designed as a microporous, mesoporous and/or macroporous metallic electrode, as a sintered electrode, as a polymer-bonded electrode or also as an electrode made of electrically conductive plastic, with preference being given to using polymer-bonded electrodes with carbon, silver or manganese as the electrically conductive catalyst .
  • an anolyte 8 is fed into the anode compartment 10 in the form of an anolyte feed 12 , which consists essentially of water, and is removed from the anode compartment 10 as an anolyte return 11 .
  • a catholyte 4 is fed into the cathode chamber 20 in the form of a catholyte feed 7 and is removed from this as a catholyte return 5 .
  • the catholyte feed 7 contains an aqueous base, for example a sodium carbonate, sodium hydroxide or ammonia solution.
  • Gaseous carbon dioxide 2 is supplied to the gas space 30 and a raw gas 3 containing carbon monoxide is removed.
  • the anode space 10, the cathode space 20 and the gas space 30 are operated at the previously explained pressures or with the explained pressure differences.
  • the carbon monoxide which is removed from the gas space 30 with the raw gas 3, is formed from the gaseous carbon dioxide 2 in a reaction that has already been described above, in that electrons are removed from the gas diffusion electrode K.
  • a first part of the carbon dioxide 2 penetrates into the gas diffusion electrode K and comes into contact there with the electrically conductive catalyst to which a negative electrical potential is applied.
  • carbon dioxide is reduced to carbon monoxide.
  • an oxygen anion is formally formed, which passes over the catholyte 4 on the opposite side of the gas diffusion electrode K and is stabilized there as hydroxide ion in the solution.
  • the gas diffusion electrode K is not absolutely gas-tight on the side with which it borders the cathode compartment, a second part of the carbon dioxide 2 can pass into the cathode compartment 20 and there either in the form of bubbles, as dissolved carbonic acid or as carbonate ions in the catholyte 4 be included.
  • This second part of the carbon dioxide 2 is consequently at least partially removed together with the catholyte 4 receiving it in the catholyte return flow 5 from the cathode space 20 and fed to a gas separator T1.
  • the carbon dioxide entrained in the catholyte return 5 is at least partially separated off in the gas separator T1 and returned as carbon dioxide recyclate 6 to the gaseous carbon dioxide 2 and thus to the gas space 30 .
  • the remaining (liquid) part of the catholyte return 5 is returned to the catholyte feed 7 after the carbon dioxide recyclate 6 has been separated off. It can thereby be ensured that the composition of the catholyte 4 remains stable over the service life of the electrolysis device 100 .
  • the recycling of the carbon dioxide recyclate 6 into the gas space 30 means that the need for fresh carbon dioxide 1 is minimized, as a result of which the method can be operated with maximum resource efficiency.
  • an electrical potential which is positive relative to the gas diffusion electrode K is applied to an anode A arranged at a distance from the membrane M in the anode chamber 10 .
  • oxygen from the water contained in the anolyte 8 is oxidized to form molecular oxygen, the excess electrons being released to the anode and the protons remaining from the water being initially dissolved in the anolyte 8 .
  • the oxygen formed is taken up in gaseous form in the form of bubbles and/or dissolved in the anolyte 8 and removed together with this in the anolyte return line 11 from the anode space.
  • the anolyte return 11 is fed to a second gas separator T2, where the oxygen entrained in it is at least partially separated off in gaseous form.
  • the remaining liquid portion of the anolyte return 11 is returned to the anolyte feed 12 .
  • the protons formed during the electrolytic water splitting and dissolved in the anolyte 8 diffuse due to the concentration gradient in the direction of the basic catholyte 4, since the membrane 4, as already mentioned, is a PEM in the exemplary embodiment shown, which allows protons to pass through. The protons can therefore get into the catholyte 4 and recombine with the hydroxide ions present there to form water.
  • the oxygen separated off in the second gas separator T2 is discharged from the electrolysis device 100 as anode gas 9 and is thus withdrawn from the process.
  • a control valve V is opened at least partially and/or at least temporarily in order to allow the anode gas 9 to flow out.
  • a measuring device can be provided, which can include a number of pressure measuring devices and optionally an evaluation device P, for example.
  • valves V, W are then opened, closed or set to a variable degree of opening, for example to set a pressure difference between the cathode space 20 and the anode space 20 .
  • the carbon dioxide recyclate 6 can be fed back into the gas space via a check valve, so that no mechanical compressors are required.
  • a counter-pressure can be overcome by appropriate design and operation of the gas separator T1.
  • the fresh charge 1 can be fed as a gas cushion via the separator T 1 and fed into the electrolysis with the carbon dioxide recyclate 6 (not shown in the figure).
  • a defined differential pressure between the cathode chamber 20 and the gas chamber 30 can be adjusted via a valve. This has the particular advantage that pressure fluctuations in the fresh insert 1 do not have a direct effect on the gas space pressure, but can be at least partially compensated for via the valve.
  • valves, measuring devices and other components can also be provided in the electrolysis device, which facilitate the feasibility of the method and the controllability or regulation of the electrolysis device.
  • Such components can be, for example, agitators and heating elements, which accelerate the separation of the gaseous components from the anolyte 11 or catholyte return 5, a raw gas treatment unit, the carbon monoxide contained in the raw gas 3 and / or hydrogen from not converted in the electrolysis Separating input gases such as carbon dioxide 2 and returning the unreacted carbon dioxide to the gas space 30, further valves and/or measuring and control devices, pumps and/or compressors or expanders and gas mixers.
  • the gaseous carbon dioxide contains inert gas components such as nitrogen and/or argon and other electrolyzable components such as steam.

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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)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Inorganic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)

Abstract

L'invention concerne un procédé de production de monoxyde de carbone à partir de dioxyde de carbone par électrolyse de dioxyde de carbone, dans lequel une unité d'électrolyse (100) est utilisée, comprenant une chambre d'anode (10) ayant une anode (A), une chambre de cathode (20) séparée de la chambre d'anode (10) par une membrane conductrice d'ions (M), et une chambre à gaz (30) séparée de la chambre de cathode (20) par une électrode de diffusion de gaz (K), la chambre d'anode (10) étant actionnée à une pression de chambre d'anode, la chambre de cathode (20) étant actionnée à une pression de chambre de cathode, et la chambre à gaz (30) étant actionnée à une pression de chambre à gaz, la chambre d'anode (10) étant alimentée en un anolyte liquide (8), la chambre de cathode (20) étant alimentée en un catholyte liquide (4) et la chambre à gaz (30) étant alimentée en dioxyde de carbone gazeux (2), une première partie du dioxyde de carbone (2) étant convertie en monoxyde de carbone au niveau de l'électrode de diffusion de gaz (K), et une seconde partie du dioxyde de carbone (2) fournie à la chambre à gaz (30) étant transférée dans le catholyte (4) par l'intermédiaire de l'électrode de diffusion de gaz (K), déchargée au moins partiellement avec le catholyte (4) hors de la chambre de cathode (20), retirée du catholyte, et renvoyée dans la chambre à gaz (30). La pression de la chambre à gaz est dans une plage comprise entre une valeur inférieure de 100 kPa à la pression de la chambre de cathode et une valeur supérieure de 10 kPa à la pression de la chambre de cathode, et l'élimination au moins partielle du dioxyde de carbone du catholyte (4) et le retour au moins partiel du dioxyde de carbone dans la chambre à gaz (30) sont effectués sans compression mécanique. L'invention concerne également un système (100) pour la mise en œuvre d'un procédé de ce type.
PCT/EP2021/025225 2020-07-30 2021-06-22 Maintien de pression dans un système d'électrolyse WO2022022849A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102020004630.4A DE102020004630A1 (de) 2020-07-30 2020-07-30 Druckhaltung in einer Elektrolyseanlage
DE102020004630.4 2020-07-30

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WO2022022849A1 true WO2022022849A1 (fr) 2022-02-03

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Cited By (2)

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Publication number Priority date Publication date Assignee Title
CN115259486A (zh) * 2022-06-30 2022-11-01 南通理工学院 一种电解法处理船舶污水的系统
EP4276223A1 (fr) * 2022-05-09 2023-11-15 Siemens Energy Global GmbH & Co. KG Mode de fonctionnement d'électrolyse de dioxyde de carbone

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WO2016124300A1 (fr) 2015-02-06 2016-08-11 Siemens Aktiengesellschaft Procédé et système d'électrolyse pour le recyclage du dioxyde de carbone
WO2016128323A1 (fr) 2015-02-09 2016-08-18 Siemens Aktiengesellschaft Procédé de réduction et système d'électrolyse permettant le recyclage électrochimique du dioxyde de carbone
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DE102016211822A1 (de) * 2016-06-30 2018-01-04 Siemens Aktiengesellschaft Anordnung und Verfahren für die Kohlendioxid-Elektrolyse
WO2019015919A1 (fr) * 2017-07-18 2019-01-24 Siemens Aktiengesellschaft Co2-électrolyseur

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WO2016128323A1 (fr) 2015-02-09 2016-08-18 Siemens Aktiengesellschaft Procédé de réduction et système d'électrolyse permettant le recyclage électrochimique du dioxyde de carbone
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DE102016211822A1 (de) * 2016-06-30 2018-01-04 Siemens Aktiengesellschaft Anordnung und Verfahren für die Kohlendioxid-Elektrolyse
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Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP4276223A1 (fr) * 2022-05-09 2023-11-15 Siemens Energy Global GmbH & Co. KG Mode de fonctionnement d'électrolyse de dioxyde de carbone
WO2023220520A1 (fr) * 2022-05-09 2023-11-16 Siemens Energy Global GmbH & Co. KG Mode de fonctionnement d'électrolyse du dioxyde de carbone
CN115259486A (zh) * 2022-06-30 2022-11-01 南通理工学院 一种电解法处理船舶污水的系统
CN115259486B (zh) * 2022-06-30 2023-05-12 南通理工学院 一种电解法处理船舶污水的系统

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