US20200318247A1 - Method and Device for the Electrochemical Utilization of Carbon Dioxide - Google Patents

Method and Device for the Electrochemical Utilization of Carbon Dioxide Download PDF

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Publication number
US20200318247A1
US20200318247A1 US16/305,302 US201716305302A US2020318247A1 US 20200318247 A1 US20200318247 A1 US 20200318247A1 US 201716305302 A US201716305302 A US 201716305302A US 2020318247 A1 US2020318247 A1 US 2020318247A1
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cathode
space
anode
carbon dioxide
cation
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Elvira María Fernández Sanchis
Marc Hanebuth
Harald Landes
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Siemens Energy Global GmbH and Co KG
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Siemens AG
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Publication of US20200318247A1 publication Critical patent/US20200318247A1/en
Assigned to Siemens Energy Global GmbH & Co. KG reassignment Siemens Energy Global GmbH & Co. KG ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: SIEMENS AKTIENGESELLSCHAFT
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    • C25B3/04—
    • 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
    • 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
    • C25B11/035—
    • C25B11/0447—
    • 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
    • C25B3/00—Electrolytic production of organic compounds
    • C25B3/20—Processes
    • C25B3/25—Reduction
    • C25B9/10—
    • 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 present disclosure relates to electrochemistry.
  • Various embodiments may include methods and electrolyzer for electrochemical utilization of carbon dioxide.
  • Some electrolysis units include a low-temperature electrolyzer in which carbon dioxide as reactant gas is converted in a cathode space 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.
  • use of an aqueous electrolyte can result not only in the formation of products of value but also disadvantageously in the formation of hydrogen, since the water in the aqueous electrolyte is likewise electrolyzed.
  • the conductivity of the electrolyte within the gap is therefore increased by adding a base or a conductive salt. It is possible for hydroxide ions to form in the non-acidic medium in the reduction of carbon dioxide at the cathode. These form hydrogencarbonate or carbonate with further carbon dioxide. Together with the cations of the base or the cations of the conductive salt, this may lead to sparingly soluble substances that precipitate out within the electrolysis cell in solid form. This may lead to a shortened lifetime of the electrolysis cell. Fundamentally, a gap in the electrolysis cell may create a drop in voltage across the cell; a rise in the energy required by the electrolysis cell leads to a drop in efficiency.
  • a further means of suppressing the unwanted formation of hydrogen is the choice of a suitable cathode material.
  • the cathode material should show maximum overvoltage for the formation of hydrogen.
  • metals of this kind are frequently toxic or lead to adverse environmental effects. Suitable metals are cadmium, mercury, and thallium.
  • the selection of these metals as cathode material restricts the selection of products of value: the product of value which is prepared in the carbon dioxide electrolysis cell depends to a crucial degree on the reaction mechanism, which is in turn affected by the cathode material as a central factor.
  • teachings of the present disclosure may be embodied in an electrolyzer and/or a method of operating an electrolyzer, in which the formation of hydrogen is reduced and the efficiency is simultaneously increased.
  • some embodiments may include an electrolyzer for electrochemical utilization of carbon dioxide, comprising at least one electrolysis cell ( 1 ), where the electrolysis cell ( 1 ) comprises an anode space ( 3 ) having an anode ( 5 ) and a cathode space ( 2 ) having a cathode ( 6 ), a first cation-permeable membrane ( 4 ) is disposed between the anode space ( 3 ) and the cathode space ( 2 ) and the anode ( 5 ) directly adjoins the first membrane ( 4 ), characterized in that a layer ( 7 ) comprising an anion-selective polymer is disposed between the first membrane ( 4 ) and the cathode ( 6 ) and where the layer ( 7 ) covers the cathode ( 6 ) at least partly but not completely.
  • a surface area of the first membrane ( 4 ) within a range from 20% to 85% is covered by the layer.
  • the cathode ( 6 ) comprises at least one of the elements silver, copper, lead, indium, tin or zinc.
  • the cathode ( 6 ) comprises a gas diffusion electrode.
  • some embodiments may include a method of operating an electrolyzer for electrochemical utilization of carbon dioxide, comprising the following steps: providing an electrolyzer having at least one electrolysis cell ( 1 ), where the electrolysis cell ( 1 ) comprises an anode space ( 3 ) having an anode ( 5 ) and a cathode space ( 2 ) having a cathode ( 6 ), and a first cation-permeable membrane ( 4 ) is disposed between the anode space ( 3 ) and the cathode space ( 2 ) and the anode ( 5 ) directly adjoins the first membrane ( 4 ), characterized in that a layer ( 7 ) comprising an anion-selective polymer is disposed between the first membrane ( 4 ) and the cathode ( 6 ), decomposing carbon dioxide to give a product at the cathode ( 6 ) in the cathode space ( 2 ), forming carbonate or hydrogencarbonate from unconverted carbon dioxide and hydroxide ions (OH
  • the electrolyzer is operated with pure water.
  • At least one of the products carbon monoxide, ethylene or formic acid is produced.
  • some embodiments may include a method of manufacturing an electrolyzer having an anion-selective polymer layer ( 7 ) at the cathode ( 6 ), wherein the cathode ( 6 ) is impregnated with the anion-selective polymer.
  • the FIGURE shows an electrolysis cell having a cathode, an anion-selective polymer layer and an anode.
  • the FIGURE shows concentration profiles of protons and hydroxide ions for operation with pure water.
  • an electrolyzer for electrochemical utilization of carbon dioxide comprises at least one electrolysis cell, where the electrolysis cell comprises an anode space having an anode and a cathode space having a cathode.
  • a first cation-permeable membrane is disposed between the anode space and the cathode space and the anode directly adjoins the first membrane.
  • a layer comprising an anion-selective polymer is disposed between the first membrane and the cathode.
  • a method for operation of an electrolyzer for electrochemical utilization of carbon dioxide the following steps are conducted: firstly, an electrolyzer having at least one electrolysis cell is provided, where the electrolysis cell comprises an anode space having an anode and a cathode space having a cathode.
  • a first cation-permeable membrane is disposed between the anode space and the cathode space. The anode directly adjoins the first membrane.
  • a layer comprising an anion-selective polymer is disposed between the first membrane and the cathode. This layer serves as a contact mediator between the first membrane and the cathode.
  • carbon dioxide is decomposed to give a product at the cathode in the cathode space.
  • Carbonate or hydrogencarbonate is then formed from unconverted carbon dioxide and hydroxide ions at the cathode.
  • hydrogen ions are transported from the anode through the first membrane.
  • the hydrogen ions and the carbonate or hydrogencarbonate then react in a contact region of the layer and the first membrane to give carbon dioxide and water.
  • the carbon dioxide can be released from the electrolysis cell through flow channels or pores in the layer.
  • the effect of the anion-selective polymer in the first layer is to exclude cations and allow only anions to pass through. This is implemented by means of immobilized positively charged ions. Typically, quaternary amines NH 4 + are immobilized. The total charge of the anion-selective layer is compensated for by mobile anions dissolved in the aqueous phase of the electrolysis cell, especially hydroxide ions, but also hydrogencarbonate ions.
  • the anion-selective layer prevents hydrogen protons in particular from getting to the cathode.
  • the unwanted formation of hydrogen is thus advantageously avoided.
  • the selection of a cathode material depends on the product of value desired.
  • the cation-permeable membrane may be implemented by means of immobilized negative charges, especially by deprotonated sulfonic acid groups. The charge is then balanced by protons or other dissolved cations, if present.
  • An unwanted but unavoidable effect in the utilization of the anion-selective layer is that some of the carbon dioxide supplied reacts with the hydroxide ions at the cathode to give carbonate or hydrogencarbonate.
  • This hydrogencarbonate or carbonate can be transported through the anion-selective layer. In contact with the hydrogen protons that can pass through the cation-permeable membrane, the hydrogencarbonate or carbonate reacts to give carbon dioxide.
  • the layer covers the cathode at least partly but not completely.
  • the carbon dioxide thus formed can escape from the electrolysis cell.
  • the partial coverage of the layer is effected in an island-like manner on the membrane.
  • the polymer layer can cover the cathode in a coherent manner when sufficient porous structures are present in the layer to allow the carbon dioxide to escape from the electrolysis cell.
  • the carbon dioxide thus formed then passes into the cathode space, where it can in turn be converted to product of value.
  • the yield of carbon dioxide in the electrolysis cell is thus increased.
  • an excess of water forms at the contact site of the anion-selective layer with the cation-selective membrane as a result of occurrence of neutralization reactions of the carbon dioxide formed from hydrogencarbonate and protons. This water formed can escape in the cathode space direction, and hence ensures good and homogeneous moistening.
  • the surface of the first membrane is covered by the layer within a range from 20% up to 85%. Within this range, it is assured that the polymer layer will separate the cathode from the cation-permeable membrane, but there are simultaneously channels or pores present to allow the carbon dioxide and water to escape.
  • This range relates to layers comprising a nonporous polymer.
  • the layer comprises a porous polymer.
  • the surface of the first membrane may be up to 100% covered, i.e. completely covered, by 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 enables a selection of the products of value formed in the electrolysis cell. More particularly, carbon monoxide can be prepared when a silver cathode is used, ethylene when a copper catalyst is used, and formic acid when a lead cathode is used.
  • the cathode comprises a gas diffusion electrode.
  • a gas diffusion electrode is understood to mean a porous catalyst structure of good electron conductivity that has been partly wetted by the adjoining membrane material. Remaining pore spaces are open to the gas side in the gas diffusion electrode.
  • the gas diffusion electrode advantageously enables the diffusing-in of carbon dioxide and the diffusing of the carbon monoxide out of the electrode, and ensures that the yield of carbon monoxide is advantageously elevated as a result.
  • the carbon dioxide released, as well as the water, is guided back into the cathode space as reactant.
  • the carbon dioxide released when a gas diffusion electrode is used, the carbon dioxide released can diffuse through the gas diffusion electrode back into the cathode space. Recycling via an external conduit is additionally possible, but is not absolutely necessary.
  • the electrolyzer is operated with pure water.
  • Pure water is understood to mean water having a conductivity of less than 1 mS/cm.
  • the use of pure water avoids precipitation of salts or carbonates during the electrolysis. In some embodiments, this prolongs the lifetime and increases the efficiency of the electrolysis cell.
  • Some embodiments include a method for production of an electrolyzer having an anion-selective polymer layer at the cathode, the cathode is impregnated with anion-selective polymer.
  • the impregnation is effected via a dipping method or by spraying the cathode with anion-selective polymer.
  • the FIGURE shows a working example of an electrolyzer with an electrolysis cell 1 , a cathode space 2 , and an anode space 3 .
  • anode space 3 there is a cation-selective membrane 4 , onto which has been directly mounted an anode 5 .
  • the cation-selective membrane 4 is cation-selective especially by virtue of the immobilizing of negative charges, in this example by means of deprotonated sulfonic acid groups, meaning that predominantly cations can pass through the membrane.
  • the anion-selective polymer 7 onto which has been directly mounted the cathode 6 . It is a feature of the anion-selective polymer that it has been modified with quaternary amines NR 4 + , such that predominantly negatively charged ions can pass through this layer.
  • the electrolysis cell 1 there is pure water as electrolyte. Carbon dioxide is decomposed at the cathode 6 , and hydroxide ions OH ⁇ form together with water. The hydroxide ions OH ⁇ can penetrate the anion-selective polymer, typically in the form of layer 7 .
  • the FIGURE shows the concentration profile of hydroxide ions OH ⁇ and protons H + in the cell.
  • the water is decomposed at the anode 5 to give 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 is also shown by the concentration profile of the protons H.
  • the carbon dioxide can diffuse back into the cathode space 2 , where it can be reused as reactant. In some embodiments, this increases the yield of the electrolysis cell 1 .
  • this electrolysis cell 1 is much higher than in the case of comparable electrolysis cells having a gap.
  • the cathode has to be divided from the cation-selective membrane in order to avoid unwanted hydrogen production.
  • the anion-selective polymer layer 7 now advantageously enables omission of this gap. In some embodiments, this increases the efficiency of the electrolysis cell since the conductivity of the electrolysis cell is distinctly increased. This likewise enables the use of pure water. In some embodiments, the use of pure water reduces the risk of precipitation of salts or carbonates. This precipitation shortens the lifetime of the electrolysis cell. Thus, the use of pure water prolongs the lifetime of the electrolysis cell.
  • the cathode 6 comprises a gas diffusion electrode comprising silver. This enables the preparation of carbon monoxide. This is especially of interest when synthesis gas is to be produced.
  • the use of pure water enables high faraday efficiencies, such that target products can be produced with maximum 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)
US16/305,302 2016-05-31 2017-05-10 Method and Device for the Electrochemical Utilization of Carbon Dioxide Pending US20200318247A1 (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE102016209447.5 2016-05-31
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

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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)

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US11193213B2 (en) * 2016-05-31 2021-12-07 Siemens Energy Global GmbH & Co. KG Device and method for the electrochemical utilisation of carbon dioxide
US11680327B2 (en) 2016-05-03 2023-06-20 Twelve Benefit Corporation 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

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
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

Citations (1)

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US20170321334A1 (en) * 2016-05-03 2017-11-09 Opus 12 Incorporated Reactor with advanced architecture for the electrochemical reaction of co2, co and other chemical compounds

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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
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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

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Publication number Priority date Publication date Assignee Title
US20170321334A1 (en) * 2016-05-03 2017-11-09 Opus 12 Incorporated Reactor with advanced architecture for the electrochemical reaction of co2, co and other chemical compounds

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US11680327B2 (en) 2016-05-03 2023-06-20 Twelve Benefit Corporation Reactor with advanced architecture for the electrochemical reaction of CO2, CO and other chemical compounds
US11193213B2 (en) * 2016-05-31 2021-12-07 Siemens Energy Global GmbH & Co. KG Device and method for the electrochemical utilisation of carbon dioxide
US11680328B2 (en) 2019-11-25 2023-06-20 Twelve Benefit Corporation Membrane electrode assembly for COx reduction

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AU2017275426B2 (en) 2019-11-14
CN109196143B (zh) 2020-10-30
AU2017275426A1 (en) 2018-11-01
EP3414363B1 (de) 2020-08-12
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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