EP3414363B1 - Verfahren und vorrichtung zur elektrochemischen nutzung von kohlenstoffdioxid - Google Patents

Verfahren und vorrichtung zur elektrochemischen nutzung von kohlenstoffdioxid Download PDF

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Publication number
EP3414363B1
EP3414363B1 EP17725540.3A EP17725540A EP3414363B1 EP 3414363 B1 EP3414363 B1 EP 3414363B1 EP 17725540 A EP17725540 A EP 17725540A EP 3414363 B1 EP3414363 B1 EP 3414363B1
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EP
European Patent Office
Prior art keywords
cathode
layer
membrane
carbon dioxide
anode
Prior art date
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EP17725540.3A
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German (de)
English (en)
French (fr)
Other versions
EP3414363A1 (de
Inventor
Harald Landes
Elvira María FERNÁNDEZ SANCHIS
Marc Hanebuth
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Siemens Energy Global GmbH and Co KG
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Siemens AG
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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
    • 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
    • C25B3/00—Electrolytic production of organic compounds
    • C25B3/20—Processes
    • C25B3/25—Reduction
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
    • C25B11/03—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form perforated or foraminous
    • C25B11/031—Porous electrodes
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/04—Electrodes; Manufacture thereof not otherwise provided for characterised by the material
    • C25B11/051—Electrodes formed of electrocatalysts on a substrate or carrier
    • C25B11/073—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material
    • C25B11/075—Electrodes formed of electrocatalysts on a substrate or carrier characterised by the electrocatalyst material consisting of a single catalytic element or catalytic compound
    • 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
    • C25B13/00—Diaphragms; Spacing elements
    • C25B13/04—Diaphragms; Spacing elements characterised by the material
    • C25B13/08—Diaphragms; Spacing elements characterised by the material based on organic materials
    • 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 an electrolyser for the electrochemical use of carbon dioxide.
  • WO 2016/039999 A1 discloses a carbon dioxide electrolyzer and a method of operating a carbon dioxide electrolyzer.
  • An advantageous design of an electrolysis unit is a low-temperature electrolyser in which carbon dioxide is converted into a cathode compartment as the reactant gas with the aid of a gas diffusion electrode.
  • the carbon dioxide is reduced to products of value at a cathode of the electrochemical cell and water is oxidized to oxygen at an anode. Due to diffusion limitations on the cathode
  • an aqueous electrolyte in addition to the formation of valuable products, the formation of hydrogen can also disadvantageously occur, since the water of the aqueous electrolyte is also electrolyzed.
  • the formation of hydrogen is further promoted if a proton-conducting membrane touches the cathode directly.
  • An alternative to this is to arrange a gap filled with aqueous electrolyte between the proton-conducting membrane and the cathode.
  • pure water cannot be used as the electrolyte, since the conductivity of the water would be too low and would result in a disadvantageously high voltage drop in the gap.
  • the use of a mineral acid, in particular dilute sulfuric acid also leads to the undesired formation of hydrogen, since these acids disadvantageously increase the proton concentration at the cathode.
  • the conductivity of the electrolyte is therefore often increased within the gap in which a base or a conductive salt is added.
  • hydroxide ions can form on the cathode during the reduction of carbon dioxide. These form hydrogen carbonate or carbonate with further carbon dioxide.
  • this disadvantageously leads to poorly soluble substances which precipitate as solids within the electrolysis cell.
  • This disadvantageously leads to a shortened service life of the electrolytic cell.
  • a gap in the electrolytic cell is disadvantageous because of the voltage drop across the cell, since the energy requirement of the electrolytic cell increases and thus the efficiency decreases.
  • cathode material Another possibility in the prior art to suppress the undesired formation of hydrogen is the choice of a suitable cathode material.
  • the cathode material should then have the highest possible overvoltage for the formation of hydrogen.
  • metals are often disadvantageously toxic or lead to negative environmental influences. Suitable metals are cadmium, mercury and thallium.
  • choosing these metals as cathode material has the disadvantage that the selection of valuable products is severely restricted: The valuable product that is produced in the carbon dioxide electrolysis cell depends largely on the reaction mechanism, on which the cathode material in turn has a central influence.
  • the object of the invention is accordingly to provide an electrolyzer and a method for operating an electrolyzer in which the formation of hydrogen is reduced and at the same time the efficiency is increased.
  • the object of the invention is achieved with an electrolyser according to claim 1 and a method for operating an electrolyser according to claim 5.
  • the electrolyser according to the invention for the electrochemical use of carbon dioxide comprises at least one electrolysis cell, the electrolysis cell comprising an anode compartment with an anode and a cathode compartment with a cathode.
  • a first cation-permeable membrane is arranged between the anode space and the cathode space and the anode is directly adjacent to this first membrane.
  • a layer comprising an anion-selective polymer is arranged between the first membrane and the cathode.
  • an electrolyser with at least one electrolysis cell comprising an anode compartment with an anode and a cathode compartment with a cathode.
  • a first cation-permeable membrane is arranged between the anode compartment and the cathode compartment.
  • the anode is directly adjacent to the first membrane.
  • a is between the first membrane and the cathode Anion-selective polymer comprising layer arranged. This layer serves as a contact mediator between the first membrane and the cathode.
  • the next step is the decomposition of carbon dioxide into a product at the cathode in the cathode compartment.
  • Carbonate or hydrogen carbonate is then formed at the cathode from unreacted carbon dioxide and hydroxide ions.
  • hydrogen ions are transported from the anode through the first membrane.
  • the hydrogen ions and the carbonate or hydrogen carbonate then react in a contact area of the layer with the first membrane to form carbon dioxide and water.
  • the carbon dioxide can be released from the electrolysis cell via flow channels or pores in the layer.
  • the anion-selective polymer of the first layer advantageously leads to the exclusion of cations and only allowing anions to pass. This is realized by immobilized positively charged ions. Quaternary amines NR 4 + are typically immobilized.
  • the overall charge of the anion-selective layer is balanced by mobile anions that are dissolved in the aqueous phase of the electrolysis cell, in particular hydroxide ions but also hydrogen carbonate ions.
  • the anion-selective layer advantageously prevents hydrogen protons in particular from reaching the cathode.
  • the undesired formation of hydrogen is thus advantageously avoided.
  • the choice of the cathode material is flexible because the anion-selective layer already prevents hydrogen protons from reaching the cathode directly.
  • the cathode material can thus advantageously be selected depending on the desired product of value.
  • the cation-permeable membrane is typically realized by immobilized negative charges, in particular by deprotonated sulfonic acid groups. The charge is then balanced by protons or other dissolved cations, if present.
  • An undesirable but unavoidable effect when using the anion-selective layer is that part of the carbon dioxide offered reacts with the hydroxide ions on the cathode to form carbonate or hydrogen carbonate.
  • This hydrogen carbonate or carbonate can be transported through the anion-selective layer.
  • the hydrogen protons which can pass through the cation-permeable membrane, the hydrogen carbonate or the carbonate reacts to form carbon dioxide.
  • the layer covers the cathode at least partially but not completely. This has the advantage that the resulting carbon dioxide can escape from the electrolysis cell.
  • the partial covering of the layer takes place similar to islands on the membrane.
  • the polymer layer can continuously cover the cathode if there are sufficient porous structures in the layer to allow the carbon dioxide to escape from the electrolysis cell. The carbon dioxide formed in this way then reaches the cathode compartment where it can in turn be converted into a valuable product.
  • the yield of carbon dioxide in the electrolysis cell is advantageously increased in this way. Furthermore, this arrangement of the electrolytic cell has the advantage that when the electrolytic cell is operated with pure water at the contact point of the anion-selective layer with the cation-selective membrane, an excess of water is created by neutralization reactions of the carbon dioxide from hydrogen carbonate and protons. This resulting water can escape in the direction of the cathode compartment and thus ensures good and even humidification.
  • the surface of the first membrane is covered by the layer in a range from 20% to 85%.
  • the polymer layer separates the cathode from the cation-permeable membrane, however channels or pores are present at the same time in order to advantageously allow the carbon dioxide and water to escape.
  • This area refers to layers that comprise a non-porous polymer.
  • the layer it is possible for the layer to comprise a porous polymer.
  • the surface of the first membrane can be covered up to 100%, that is to say completely, with the layer, since carbon dioxide and water can then escape through pores.
  • the cathode comprises at least one of the elements silver, copper, lead, indium, tin or zinc.
  • the selection of the cathode material advantageously enables a selection of the products of value that arise in the electrolysis cell.
  • a silver cathode is used, carbon monoxide can be produced, if a copper cathode is used, ethylene can be produced, and if a lead cathode is used, formic acid.
  • the cathode comprises a gas diffusion electrode.
  • a gas diffusion electrode is understood to be an electronically conductive, porous catalyst structure that is partially wetted with the adjacent membrane material. Remaining pore spaces are open on the gas side of the gas diffusion electrode.
  • the gas diffusion electrode advantageously enables the carbon dioxide to diffuse in and the carbon monoxide to diffuse out of the electrode and ensures that the yield of the carbon monoxide is thereby advantageously increased.
  • the released carbon dioxide in addition to the water, is fed back into the cathode space as an educt.
  • the released carbon dioxide can advantageously diffuse back into the cathode space through the gas diffusion electrode.
  • the return via an external line can also take place, but is not absolutely necessary.
  • the electrolyzer is operated with pure water.
  • Pure water is understood to mean water that has a conductivity of less than 1 mS / cm.
  • the use of pure water advantageously prevents salts or carbonates from precipitating during the electrolysis. This advantageously extends the service life and increases the efficiency of the electrolysis cell.
  • Figure 1 shows an electrolysis cell with a cathode, an anion-selective polymer layer and an anode. Furthermore shows Figure 1 Concentration profiles of protons and hydroxide ions for operation with pure water.
  • Figure 1 shows an embodiment of the electrolyser with an electrolysis cell 1, a cathode compartment 2 and an anode compartment 3.
  • anode compartment 3 there is a cation-selective membrane 4 to which an anode 5 is applied directly.
  • the cation-selective membrane 4 is cation-selective in particular due to the immobilization of negative charges, in this example by means of deprotonated sulfonic acid groups, ie that predominantly cations can pass through the membrane.
  • the anion-selective polymer 7 to which the cathode 6 is applied directly is located in the cathode compartment 2.
  • the anion-selective polymer is characterized by the fact that it has Quaternary amines NR 4 + was modified so that predominantly negatively charged ions can pass through this layer.
  • Pure water is present as an electrolyte in the electrolytic cell 1.
  • Carbon dioxide is broken down at the cathode 6 and hydroxide ions OH - are formed together with water.
  • the hydroxide ions OH - can penetrate the anion-selective polymer, which is typically designed as layer 7.
  • Figure 1 the concentration profile of hydroxide ions OH - and protons H + in the cell is shown.
  • the water is broken down at the anode 5 into protons and oxygen.
  • the oxygen can leave the electrolysis cell 1 via the anode space 3.
  • the protons H + can cross the cation-selective membrane 4. This also shows the concentration profile of the protons H + .
  • the efficiency of this electrolysis cell 1 is significantly higher than that of comparable electrolysis cells with a gap.
  • the cathode In electrolytic cells with a gap, the cathode must be separated from the cation-selective membrane in order to avoid undesired hydrogen production.
  • the anion-selective polymer layer 7 now advantageously makes it possible to omit this gap. This advantageously increases the efficiency of the electrolytic cell, since the conductivity of the electrolytic cell is significantly increased.
  • This also enables the use of pure water.
  • the use of pure water advantageously reduces the risk of precipitation of salts or carbonates. This failure shortens the life of the electrolytic cell. Thus, the use of pure water extends the life of the electrolysis cell.
  • the cathode 6 comprises a gas diffusion electrode comprising silver. This enables carbon monoxide to be produced. This is of particular interest when synthesis gas is to be produced. The use of pure water enables high Faraday efficiencies, so that target products can be manufactured with the greatest possible purity at low voltage.

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Inorganic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)
EP17725540.3A 2016-05-31 2017-05-10 Verfahren und vorrichtung zur elektrochemischen nutzung von kohlenstoffdioxid Active EP3414363B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102016209447.5A DE102016209447A1 (de) 2016-05-31 2016-05-31 Verfahren und Vorrichtung zur elektrochemischen Nutzung von Kohlenstoffdioxid
PCT/EP2017/061185 WO2017207232A1 (de) 2016-05-31 2017-05-10 Verfahren und vorrichtung zur elektrochemischen nutzung von kohlenstoffdioxid

Publications (2)

Publication Number Publication Date
EP3414363A1 EP3414363A1 (de) 2018-12-19
EP3414363B1 true EP3414363B1 (de) 2020-08-12

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EP17725540.3A Active EP3414363B1 (de) 2016-05-31 2017-05-10 Verfahren und vorrichtung zur elektrochemischen nutzung von kohlenstoffdioxid

Country Status (8)

Country Link
US (1) US20200318247A1 (zh)
EP (1) EP3414363B1 (zh)
CN (1) CN109196143B (zh)
AU (1) AU2017275426B2 (zh)
DE (1) DE102016209447A1 (zh)
DK (1) DK3414363T3 (zh)
ES (1) ES2830735T3 (zh)
WO (1) WO2017207232A1 (zh)

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CA3022807C (en) 2016-05-03 2021-08-24 Opus 12 Incorporated Reactor with advanced architecture for the electrochemical reaction of co2, co, and other chemical compounds
US11680328B2 (en) 2019-11-25 2023-06-20 Twelve Benefit Corporation Membrane electrode assembly for COx reduction
DE102016209451A1 (de) * 2016-05-31 2017-11-30 Siemens Aktiengesellschaft Vorrichtung und Verfahren zur elektrochemischen Nutzung von Kohlenstoffdioxid
CN113795611A (zh) * 2019-05-05 2021-12-14 多伦多大学管理委员会 在电解池中碳酸盐转化为合成气或c2+产物

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NL6914397A (zh) * 1968-09-28 1970-04-01
ES2132364T3 (es) * 1993-02-26 1999-08-16 Permelec Electrode Ltd Celula de electrolisis y procedimientos de produccion de hidroxido alcalino y de peroxido de hidrogeno.
GB0016379D0 (en) * 2000-07-05 2000-08-23 Johnson Matthey Plc Electrochemical cell
CN1369576A (zh) * 2001-02-16 2002-09-18 深圳市柯雷恩环境科技有限公司 反式双膜三室电解槽
US9481939B2 (en) * 2010-07-04 2016-11-01 Dioxide Materials, Inc. Electrochemical device for converting carbon dioxide to a reaction product
WO2016064440A1 (en) * 2014-10-21 2016-04-28 Dioxide Materials Electrolyzer and membranes
CN102912374B (zh) * 2012-10-24 2015-04-22 中国科学院大连化学物理研究所 一种以双极膜为隔膜的电化学还原co2电解池及其应用
KR20160019218A (ko) * 2014-08-11 2016-02-19 한국과학기술원 탄산염 및 산의 제조 방법
KR102446810B1 (ko) * 2014-09-08 2022-09-23 쓰리엠 이노베이티브 프로퍼티즈 캄파니 이산화탄소 전해조용 이온성 중합체 막
CA3022807C (en) * 2016-05-03 2021-08-24 Opus 12 Incorporated Reactor with advanced architecture for the electrochemical reaction of co2, co, and other chemical compounds

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Also Published As

Publication number Publication date
AU2017275426B2 (en) 2019-11-14
CN109196143B (zh) 2020-10-30
AU2017275426A1 (en) 2018-11-01
US20200318247A1 (en) 2020-10-08
ES2830735T3 (es) 2021-06-04
DE102016209447A1 (de) 2017-11-30
WO2017207232A1 (de) 2017-12-07
EP3414363A1 (de) 2018-12-19
DK3414363T3 (da) 2020-10-19
CN109196143A (zh) 2019-01-11

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