EP3478879A1 - Agencement et procédé pour l'électrolyse du dioxyde de carbone - Google Patents

Agencement et procédé pour l'électrolyse du dioxyde de carbone

Info

Publication number
EP3478879A1
EP3478879A1 EP17725925.6A EP17725925A EP3478879A1 EP 3478879 A1 EP3478879 A1 EP 3478879A1 EP 17725925 A EP17725925 A EP 17725925A EP 3478879 A1 EP3478879 A1 EP 3478879A1
Authority
EP
European Patent Office
Prior art keywords
cathode
gas
space
electrolyte
gas space
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.)
Withdrawn
Application number
EP17725925.6A
Other languages
German (de)
English (en)
Inventor
Savo Asanin
Van An DU
Maximilian Fleischer
Philippe Jeanty
Erhard Magori
Angelika Tawil
Kerstin Wiesner-Fleischer
Oliver von Sicard
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.)
Siemens AG
Original Assignee
Siemens AG
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 Siemens AG filed Critical Siemens AG
Publication of EP3478879A1 publication Critical patent/EP3478879A1/fr
Withdrawn legal-status Critical Current

Links

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
    • 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
    • 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
    • C25B11/032—Gas diffusion 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
    • C25B15/00—Operating or servicing cells
    • C25B15/02—Process control or regulation
    • 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
    • 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
    • C25B3/00—Electrolytic production of organic compounds
    • C25B3/20—Processes
    • C25B3/25—Reduction
    • C25B3/26—Reduction of carbon dioxide
    • 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
    • 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

  • Apparatus and method for carbon dioxide electrolysis the invention relates to an arrangement and a method for the carbon dioxide electrolysis according to the preamble of An ⁇ demanding. 1
  • metals are used as catalysts Kata ⁇ .
  • the type of metal influences the products of electrolysis. For example, CO 2 is reduced almost exclusively to CO, for example on Ag, Au, Zn, and with restrictions on Pd, Ga, whereas copper has a large number of hydrocarbons as reduction products. care is.
  • pure metals and metal alloys and mixtures of metal and metal oxide which is catalytically effective co-, of interest because they may increase the Selekti ⁇ tivity of a specific hydrocarbon.
  • a gas diffusion electrode (GDE) are used as the cathode, similar to the chlor-alkali electrolysis to Zvi ⁇ rule the liquid electrolyte, the gaseous C02 and the solid silver particles to produce a three-phase boundary.
  • GDE gas diffusion electrode
  • an electrolytic cell as known also from the fuel cell technology, used with two electrolyte compartments, the Elect ⁇ rolythuntn are separated by an ion exchange membrane.
  • the working electrode is a porous gas diffusion electrode. It comprises a metal net on which a mixture of PTFE, activated carbon, a catalyst and other components is applied. It includes a pore system into which the
  • the counter electrode is a sheet applied with platinum or an iridium mixed oxide.
  • the GDE is in contact with the electrolyte on one side. On the other hand, it is supplied with C02, which is forced through the GDE with overpressure (so-called convective mode of operation).
  • the GDE can while holding various metals and metal compounds ent ⁇ that have a catalytic effect on the process.
  • the functioning of a GDE is known, for example, from EP 297377 A2, EP 2444526 A2 and EP 2410079 A2.
  • the resulting product is gaseous and not liquid at the Koh ⁇ dioxide electrolysis. Furthermore, with the from the electrolyte ent ⁇ standing alkali or alkaline earth metal hydroxide used the C02 forming salts.
  • the electrolyte KOH the electrolyte KOH and there are the salts of KHC03 and K2C03. by virtue of The operating conditions lead to a crystallization of the salts in and on the GDE from the gas side.
  • a stable long-term operation of the gas diffusion electrode in the range of more than 1000 h is not possible in the C02 electrolysis, since the resulting salt clogs the pores of the GDE and thus this gas-impermeable. It is an object of the present invention to provide an improved arrangement for the carbon dioxide electrolysis and a method for operating an arrangement for the carbon dioxide electrolysis, with the stable long-term operation while avoiding the aforementioned disadvantages is made possible.
  • the arrangement according to the invention for the carbon dioxide electrolysis comprises an electrolysis cell with an anode and a cathode, which are both connected to a power supply.
  • the cathode is designed as a gas diffusion electrode, to which a gas space is connected on a first side and a cathode space on a second side.
  • the arrangement comprises a sequent to the electrolysis cell subse- electrolyte circulation and a gas supply for Zumoni ⁇ tion of carbon dioxide-containing gas into the gas space.
  • the gas space has an electrolyte outlet and the electrolyte outlet is provided with a shut-off device.
  • DA in the arrangement is configured such that the shut ⁇ device is opened when the pressure difference between the gas space and cathode space exceeds a threshold.
  • the shut-off device may be in particular a Absperrschie ⁇ ber, a butterfly valve or ball valve.
  • the shut-off device can be a safety valve (pressure relief valve) or a proportional valve.
  • an over ⁇ pressure valve requires no control, but opens automatically when the threshold value for the pressure difference between the gas space and the cathode space is exceeded.
  • a first pressure sensor may be present in the gas space. This is a pressure signal, for example, to a control ⁇ device for controlling the shut-off device.
  • a second pressure sensor may be arranged in the cathode compartment. This may also give a pressure signal to the controller. From the two pressure signals, the control device can determine the pressure difference and make a control of the shut-off device.
  • a differential pressure sensor for gas space and cathode space may be present. This gives directly a signal for the pressure difference to a control device or directly to the shut-off device.
  • the electrolyte outlet can be connected to the electrolyte circuit.
  • the electrolyte discharged via the shut-off device can subsequently be returned to the system.
  • the electrolyte is not consumed.
  • the C0 2 feed gas flow is not influenced in this case and thus a sufficient C0 2 supply of the process is ensured.
  • a controller may be provided securelystal- tet to control the shut-off function of the Druckdif ⁇ ference.
  • the shut-off device can be operated so that the pressure difference between the gas space and the cathode space remains within a definable interval. It remains preferred always in the gas space, a higher pressure than in the cathode compartment.
  • the interval can be narrow, so that, for example, the pressure difference does not fluctuate by more than 10% or not more than 5%.
  • an electrolysis cell 11, shown schematically in Figure 1 is typically adapted to carry out a carbon dioxide ⁇ electrolysis.
  • the guide shape of the electrolytic cell 11 at least one anode 13 with adjacent anode space 12 and a cathode 15 and egg ⁇ NEN adjacent cathode space 14.
  • Anodenraum 12 and cathode space 14 are separated by a membrane 21 from each other.
  • a construction without membrane 21 is also conceivable in which a pH compensation then exceeds that of the membrane 21.
  • Anode 13 and cathode 15 are electrically connected to a voltage supply 22, which is controlled by the control unit 23.
  • the control unit 23 can apply a protective voltage or an operating voltage to the electrodes 13, 15, that is to say the anode 13 and the cathode 15.
  • the anode compartment 12 of the electrolysis cell 11 shown is equipped with an electrolyte inlet.
  • the illustrated Ano ⁇ denraum 12 includes an outlet for electrolyte and, for example, oxygen O 2 or other gaseous by-product, which is gebil ⁇ det in the carbon dioxide electrolysis at the anode 13.
  • oxygen O 2 or other gaseous by-product which is gebil ⁇ det in the carbon dioxide electrolysis at the anode 13.
  • chloride-containing anolyte for example, chlorine gas is formed.
  • the cathode compartment 14 also has depending ⁇ wells at least one product and electrolyte outlet on. Since ⁇ the total electrolysis product can be composed of a variety of electrolysis products.
  • the electrolytic cell 11 is further designed in a three-chamber structure, in which the carbon dioxide CO 2 is flowed through the cathode 15 designed as a gas diffusion electrode in the Katho ⁇ denraum 14.
  • Gas diffusion electrodes make it possible to bring a solid catalyst th a liquid electrolytically, and a gaseous Elektrolyseedukt in contact MITEI ⁇ Nander.
  • the catalyst can be made porous and take over the electrode function, or a porous electrode takes over the catalyst function.
  • the pore system of the electrode is designed so that the liquid and the gaseous phase can equally penetrate into the pore system and present therein or at its electrically accessible surface at the same time. can.
  • An example of a gas diffusion electrode is an oxygen discharge electrode.
  • a gas diffusion electrode comprising the Ka Thode 15 in this example, a metal mesh on which a Mi ⁇ research made of PTFE, activated carbon and a catalyst is applied.
  • a metal mesh on which a Mi ⁇ research made of PTFE, activated carbon and a catalyst is applied.
  • Catholyte includes the electrolytic cell 11 is a Koh ⁇ lenstoffdioxideinlass 24 16 into the gas space, the carbon dioxide reaches the gas chamber 16, the cathode 15 and may there penetrate into the porous structure of the cathode 15 and arrive to the reaction.
  • the gas space 16 in the present example comprises an electrolyte outlet 25, which is arranged in the bottom area.
  • the electrolyte outlet 25 leads via a pressure-controlled proportional valve 32 to the reservoir 19.
  • a first pressure sensor 31 is present which measures the pressure in the gas space 16 and a second pressure sensor 30 for measuring the pressure in the cathode space 14.
  • the control device 23 receives the measurement signals of the pressure sensors 30, 31 and determines the pressure difference between the cathode chamber 14 and the gas chamber 16. If the pressure difference exceeds a definable threshold, the valve 32 is opened so that accumulated electrolyte from the gas space 16 from ⁇ run can. The electrolyte is returned to the reservoir 19. If the pressure difference falls below the threshold value or a second threshold value, the valve is closed.
  • the cathode 15 "pumped" in the direction of the gas space 16. It arises 16 drops on the surface of the cathode 15 which coalesce and collect in the form of a film in the lower portion of the cathode 15. The accumulating electrolyte thereby causes a drop
  • valve 32 By operating the valve 32 the electrolysis of all ⁇ recently is constantly operated in a certain differential pressure area between gas space 16 and the electrolyte. This will maintain the "electrolyte pump" through the cathode 15 and avoid salinisation of the gas diffusion electrode

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Automation & Control Theory (AREA)
  • Inorganic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)

Abstract

L'invention concerne un agencement pour l'électrolyse du dioxyde de carbone et un procédé pour le faire fonctionner, ledit agencement comprenant une cellule électrolytique pourvue d'une anode et d'une cathode, l'anode et la cathode étant reliées par une alimentation électrique, la cathode étant conçue en tant qu'électrode de diffusion gazeuse à laquelle est raccordé, sur une première face, un compartiment gazeux et, sur une deuxième face, un compartiment cathodique, l'agencement comprenant également un circuit électrolytique adjacent à la cellule électrolytique et une alimentation en gaz servant à acheminer un gaz contenant du dioxyde de carbone dans le compartiment gazeux. Le compartiment gazeux présente une sortie pour l'électrolyte, la sortie pour l'électrolyte est dotée d'un dispositif de fermeture, conçu de sorte que ledit dispositif de fermeture est ouvert lorsque la différence de pression entre le compartiment gazeux et le compartiment passe au-dessus d'une valeur de seuil.
EP17725925.6A 2016-06-30 2017-05-18 Agencement et procédé pour l'électrolyse du dioxyde de carbone Withdrawn EP3478879A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102016211819.6A DE102016211819A1 (de) 2016-06-30 2016-06-30 Anordnung und Verfahren für die Kohlendioxid-Elektrolyse
PCT/EP2017/061927 WO2018001637A1 (fr) 2016-06-30 2017-05-18 Agencement et procédé pour l'électrolyse du dioxyde de carbone

Publications (1)

Publication Number Publication Date
EP3478879A1 true EP3478879A1 (fr) 2019-05-08

Family

ID=58772873

Family Applications (1)

Application Number Title Priority Date Filing Date
EP17725925.6A Withdrawn EP3478879A1 (fr) 2016-06-30 2017-05-18 Agencement et procédé pour l'électrolyse du dioxyde de carbone

Country Status (6)

Country Link
US (1) US20190233958A1 (fr)
EP (1) EP3478879A1 (fr)
CN (1) CN109415830A (fr)
AU (1) AU2017291062B2 (fr)
DE (1) DE102016211819A1 (fr)
WO (1) WO2018001637A1 (fr)

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BR112020014938A2 (pt) 2018-01-22 2021-02-23 Opus-12 Incorporated sistema e método para o controle de reator de dióxido de carbono
DE102018222338A1 (de) * 2018-12-19 2020-06-25 Siemens Aktiengesellschaft Elektrolyseur zur Kohlenstoffdioxidreduktion
EP3757253A1 (fr) * 2019-06-24 2020-12-30 Siemens Aktiengesellschaft Système d'électrolyse et procédé d'accumulation de l'énergie électrique au moyen du système d'électrolyse
DE102019211942A1 (de) 2019-08-08 2021-02-11 Siemens Aktiengesellschaft Verfahren zur elektrochemischen Umsetzung eines Eduktgases an einer Gasdiffusionselektrode mit Differenzdruckermittlung
DE102019218297A1 (de) * 2019-11-26 2021-05-27 Siemens Aktiengesellschaft Elektrolyse-Anlage und Betriebsverfahren für eine Elektrolyse-Anlage zur elektrochemischen Reduktion von Kohlendioxid
US20230002919A1 (en) * 2019-12-11 2023-01-05 Nippon Telegraph And Telephone Corporation Carbon Dioxide Gas Phase Reduction Apparatus and Method
CN111575726B (zh) * 2020-05-27 2021-10-01 上海科技大学 一种用于二氧化碳的电化学还原的电化学反应器
CN111910211B (zh) * 2020-06-22 2021-11-19 西安交通大学 一种连续流动光电催化co2还原反应系统
CA3196179A1 (fr) 2020-10-20 2022-04-28 Lihui Wang Polymeres reticules et semi-interpenetrants et leurs membranes
JP7203876B2 (ja) * 2021-03-04 2023-01-13 本田技研工業株式会社 電気化学反応装置、二酸化炭素の還元方法、及び炭素化合物の製造方法
JP7520754B2 (ja) * 2021-03-15 2024-07-23 株式会社東芝 二酸化炭素電解装置及び二酸化炭素電解方法
CN113373462A (zh) * 2021-05-21 2021-09-10 南京理工大学 一种用于电化学还原co2的膜式液流电解池及测试工艺
NL2032221B1 (en) * 2022-06-20 2024-01-08 Univ Delft Tech Device for performing a biologically catalysed electrochemical reaction
US11939284B2 (en) 2022-08-12 2024-03-26 Twelve Benefit Corporation Acetic acid production

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US3410770A (en) * 1966-02-18 1968-11-12 Allis Chalmers Mfg Co Electrolytic method for producing oxygen and hydrogen
US4108742A (en) * 1974-03-09 1978-08-22 Asahi Kasei Kogyo Kabushiki Kaisha Electrolysis
DE3722019A1 (de) 1987-07-03 1989-01-12 Varta Batterie Verfahren zur herstellung einer kunststoffgebundenen gasdiffusionselektrode, die einen manganoxidkatalysator der ueberwiegenden zusammensetzung mno(pfeil abwaerts)2(pfeil abwaerts)o(pfeil abwaerts)3(pfeil abwaerts)* x mn(pfeil abwaerts)5(pfeil abwaerts)o(pfeil abwaerts)8(pfeil abwaerts) enthaelt
DE102010031571A1 (de) 2010-07-20 2012-01-26 Bayer Materialscience Ag Sauerstoffverzehrelektrode
DE102010042729A1 (de) 2010-10-21 2012-04-26 Bayer Materialscience Aktiengesellschaft Sauerstoffverzehrkathode und Verfahren zu ihrer Herstellung
US9255335B2 (en) * 2011-07-26 2016-02-09 The Board Of Trustees Of The Leland Stanford Junior University Catalysts for low temperature electrolytic CO2 reduction
CN103339293A (zh) * 2011-08-29 2013-10-02 松下电器产业株式会社 还原二氧化碳的方法
DE102013226357A1 (de) * 2013-12-18 2015-06-18 Siemens Aktiengesellschaft Pulsierende Elektrolytzufuhr in den Reaktionsraum einer Elektrolysezelle mit gasentwickelnden Elektroden

Also Published As

Publication number Publication date
US20190233958A1 (en) 2019-08-01
CN109415830A (zh) 2019-03-01
WO2018001637A1 (fr) 2018-01-04
AU2017291062A1 (en) 2018-12-13
DE102016211819A1 (de) 2018-01-18
AU2017291062B2 (en) 2019-09-19

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