US20190233957A1 - Arrangement for the Electrolysis of Carbon Dioxide - Google Patents

Arrangement for the Electrolysis of Carbon Dioxide Download PDF

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Publication number
US20190233957A1
US20190233957A1 US16/312,203 US201716312203A US2019233957A1 US 20190233957 A1 US20190233957 A1 US 20190233957A1 US 201716312203 A US201716312203 A US 201716312203A US 2019233957 A1 US2019233957 A1 US 2019233957A1
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US
United States
Prior art keywords
gas
space
cathode
electrolyte
gas space
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Abandoned
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US16/312,203
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English (en)
Inventor
Philippe Jeanty
Erhard Magori
Christian Scherer
Angelika Tawil
Kerstin Wiesner-Fleischer
Oliver von Sicard
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Siemens AG
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Siemens AG
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Assigned to SIEMENS AKTIENGESELLSCHAFT reassignment SIEMENS AKTIENGESELLSCHAFT ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: von Sicard, Oliver, TAWIL, ANGELIKA, JEANTY, PHILIPPE, MAGORI, ERHARD, SCHERER, CHRISTIAN, Wiesner-Fleischer, Kerstin
Publication of US20190233957A1 publication Critical patent/US20190233957A1/en
Abandoned legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
    • 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
    • C25B15/00—Operating or servicing cells
    • C25B15/02—Process control or regulation
    • 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
    • C25B3/00—Electrolytic production of organic compounds
    • C25B3/20—Processes
    • C25B3/25—Reduction
    • C25B9/08—
    • 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

Definitions

  • teachings of the present disclosure relate to electrolysis of carbon dioxide.
  • Various embodiments may include an arrangement for carbon dioxide electrolysis.
  • CO2 is converted to carbohydrates by photosynthesis. This complex process can be reproduced on the industrial scale only with great difficulty.
  • One currently technically feasible route is the electrochemical reduction of CO2.
  • the carbon dioxide is converted here with supply of electrical energy to a product of higher energy value, for example CO, CH4, C2H4 or C1-C4 alcohols.
  • the electrical energy in turn preferably comes from renewable energy sources such as wind power or photovoltaics.
  • metals are used as catalysts.
  • the type of metal affects the products of the electrolysis.
  • CO2 is reduced virtually exclusively to CO over Ag, Au, Zn and, to a limited degree, over Pd and Ga, whereas a multitude of hydrocarbons are observed as reduction products over copper.
  • metal alloys are also of interest, as are mixtures of metal and metal oxide having cocatalytic activity, since these can increase selectivity for a particular hydrocarbon.
  • a gas diffusion electrode In CO2 electrolysis, a gas diffusion electrode (GDE) can be used as cathode in a similar manner to that in chlor-alkali electrolysis in order to establish a three-phase boundary between the liquid electrolyte, the gaseous CO2 and the solid silver particles.
  • GDE gas diffusion electrode
  • the working electrode is a porous gas diffusion electrode. It comprises a metal mesh, to which a mixture of PTFE, activated carbon, a catalyst and further components has been applied. It comprises a pore system into which the reactants penetrate and react at the three-phase interfaces.
  • the counterelectrode is sheet metal coated with platinum or a mixed iridium oxide.
  • the GDE is in contact with the electrolyte on one side. On the other side it is supplied with CO2 which is forced through the GDE by positive pressure (called convective mode of operation).
  • the GDE here may contain various metals and metal compounds that have a catalytic effect on the process.
  • the mode of function of a GDE is known, for example, from EP 297377 A2, EP 2444526 A2 and EP 2410079 A2.
  • the product formed in carbon dioxide electrolysis is gaseous and not liquid.
  • the CO2 used forms salts with the alkali metal or alkaline earth metal hydroxide formed from the electrolyte.
  • KOH is formed, and the salts KHCO3 and K2CO3 are formed. Owing to the operating conditions, there is crystallization of the salts in and on the GDE from the gas side.
  • some embodiments may include an arrangement ( 10 ) for carbon dioxide electrolysis, comprising: an electrolysis cell ( 11 ) having an anode ( 13 ) and a cathode ( 15 ), where anode ( 13 ) and cathode ( 15 ) are connected to a voltage supply ( 22 ), where the cathode ( 15 ) takes the form of a gas diffusion electrode adjoined on a first side by a gas space ( 16 ) and on a second side by a cathode space ( 14 ), an electrolyte circuit ( 20 ) that adjoins the electrolysis cell ( 11 ), a gas supply ( 17 ) for supplying carbon dioxide-containing gas to the gas space ( 16 ), characterized in that the gas space ( 16 ) has an outlet ( 25 ) for electrolyte, carbon dioxide and product gases from the electrolysis, the outlet ( 25 ).
  • the throttle ( 30 ) comprises a pipe arranged at an angle of between 0° and 80° to the vertical.
  • the pipe is in an essentially vertical arrangement.
  • the pipe is in a rotatable arrangement.
  • the internal diameter of the pipe is at least twice, especially at least five times, the rest of the connection between gas space ( 16 ) and electrolyte circuit ( 20 ).
  • the outlet ( 25 ) is connected to the gas supply via a return connection.
  • the pump apparatus ( 27 ) is disposed in the return connection.
  • the pump apparatus ( 27 ) is disposed in the gas space ( 16 ).
  • the pressure differential between gas space ( 16 ) and cathode space ( 14 ) is kept between 10 and 100 hPa.
  • the outlet ( 25 ) in the gas space ( 16 ) is disposed at the bottom end.
  • the outlet ( 25 ) is connected to an overflow vessel ( 26 ).
  • the gas space ( 16 ) has turbulence promoters.
  • the turbulence promoters are configured such that an air gap of at least 0.1 mm remains between them and the surface of the cathode ( 15 ).
  • an arrangement for carbon dioxide electrolysis comprises an electrolysis cell having an anode and a cathode, where anode and cathode are connected to a voltage supply, where the cathode takes the form of a gas diffusion electrode adjoined on a first side by a gas space and on a second side by a cathode space, an electrolyte circuit that adjoins the electrolysis cell and a gas supply for supplying carbon dioxide-containing gas to the gas space.
  • the gas space has an outlet for electrolyte, carbon dioxide and product gases from the electrolysis and the outlet is connected via a throttle to the electrolyte circuit, where the throttle is configured so as to bring about a definable pressure differential between gas space and cathode space when a mixture of product gases and liquid electrolyte flows through it.
  • an electrolysis cell 11 shown in schematic form in the FIGURE is typically suitable for undertaking a carbon dioxide electrolysis.
  • This embodiment of the electrolysis cell 11 comprises at least one anode 13 with an adjoining anode space 12 , and a cathode 15 and an adjoining cathode space 14 .
  • Anode space 12 and cathode space 14 are separated from one another by a membrane 21 .
  • the membrane 21 is typically manufactured from a PTFE-based material. According to the electrolyte solution used, a construction without a membrane 21 is also conceivable, in which case pH balancing then goes beyond that by 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 may apply a protection voltage or an operating voltage to the electrodes 13 , 15 , i.e. the anode 13 and the cathode 15 .
  • the anode space 12 of the electrolysis cell 11 shown is equipped with an electrolyte inlet.
  • the anode space 12 depicted likewise comprises an outlet for electrolyte and, for example, oxygen O 2 or another gaseous by-product which is formed in the carbon dioxide electrolysis at the anode 13 .
  • the cathode space 14 in each case likewise has at least one product and electrolyte outlet.
  • the overall electrolysis product may be composed of a multitude of electrolysis products.
  • the electrolysis cell 11 is also executed in a three-chamber construction in which the carbon dioxide CO 2 is introduced into the cathode space 14 via the cathode 15 executed as a gas diffusion electrode.
  • Gas diffusion electrodes enable mutual contacting of a solid catalyst, a liquid electrolyte and a gaseous electrolysis reactant.
  • the catalyst may be executed in porous form and assume the electrode function, or a porous electrode assumes the catalyst function.
  • the pore system of the electrode is configured here such that the liquid phase and the gaseous phase can penetrate equally into the pore system and may be present simultaneously therein, i.e. at the electrically accessible surface thereof.
  • a gas diffusion electrode is an oxygen-depolarized electrode which is used in chloralkali electrolysis.
  • the cathode 15 in this example comprises a metal mesh to which a mixture of PTFE, activated carbon and a catalyst has been applied.
  • the electrolysis cell 11 For introduction of the carbon dioxide CO2 into the catholyte circuit, the electrolysis cell 11 comprises a carbon dioxide inlet 24 into the gas space 16 . In the gas space 16 , the carbon dioxide reaches the cathode 15 , where it can penetrate into the porous structure of the cathode 15 and hence be reacted.
  • the arrangement 10 comprises an electrolyte circuit 20 , by means of which the anode space 12 and the cathode space 14 are supplied with a liquid electrolyte, for example K2SO4, KHCO3, KOH, Cs2SO4, and the electrolyte is recycled into a reservoir 19 .
  • a liquid electrolyte for example K2SO4, KHCO3, KOH, Cs2SO4, and the electrolyte is recycled into a reservoir 19 .
  • the electrolyte is circulated in the electrolyte circuit 20 by means of an electrolyte pump 18 .
  • the gas space 16 comprises an outlet 25 disposed in the base region.
  • the outlet 25 is configured as an opening with sufficient cross section, so that both electrolyte that passes through the cathode 15 and carbon dioxide and product gases can get through the outlet into the connecting pipe.
  • the outlet 25 leads to an overflow vessel 26 .
  • the liquid electrolyte is collected and accumulates in the overflow vessel 26 .
  • Carbon dioxide and product gases that come from the gas space 16 are separated from the electrolyte and accumulate above it.
  • a further pipe 28 leads to a pump 27 , in this working example a membrane pump, and further to the gas supply 17 .
  • the pump 27 may also be a piston pump, stroke pump, extruder pump or gear pump.
  • Part of the gas supply 17 , the gas space 16 , the pipe 18 and the overflow vessel 26 together with the connection thereof to the outlet 25 thus form a circuit.
  • the pump 27 the carbon dioxide and product gases present are guided from the overflow vessel 26 back into the gas supply and hence the gas is partly circulated.
  • the volume flow rate of the pump 27 is much higher than the volume flow rate of new carbon dioxide.
  • Reactant gas that has not been consumed is thus advantageously guided once again past the cathode 15 and once or more than once has the opportunity to be reduced.
  • Product gases are likewise partly circulated here.
  • the repeated passage of the carbon dioxide past the cathode 15 increases the efficiency of the conversion.
  • This connection begins with an outlet 29 disposed at a side wall of the overflow vessel 26 , in some embodiments close to the base, but not at the base.
  • the outlet 29 is connected to a throttle 30 in the form of a vertical pipe section having a length of 90 cm, for example.
  • the diameter of this pipe section is much greater than that of the inlets to the throttle 30 .
  • the inlet has, for example, an internal diameter of 4 mm; the pipe section has an internal diameter of 20 mm.
  • the throttle 30 is connected on the outlet side, i.e. at the upper end of the pipe section, to the electrolyte circuit 20 .
  • the throttle 30 establishes and maintains a pressure differential between the electrolyte circuit 20 connected at the top end and hence also the cathode space 14 on the one hand and the overflow vessel 26 and the gas space 16 on the other hand.
  • This pressure differential is between 10 and 100 hPa (mbar), meaning that the gas space 16 remains at only slightly elevated pressure relative to the cathode space 14 .
  • the throttle 30 establishes the pressure differential irrespective of whether a liquid or gaseous medium is currently flowing through, or a mixture thereof.
  • the pressure differential is established depending on the height of the pipe section, owing to the hydrostatic pressure. If the pipe section is mounted in a rotatable manner, the pressure differential of the throttle 30 can be lowered in an infinitely variable manner, down to virtually zero in a horizontal position.
  • the electrical voltage applied to the cathode 15 results in “pumping” of electrolyte out of the catholyte space 14 through the gas diffusion electrode, i.e. the cathode 15 , in the direction of gas space 16 .
  • Droplets form on the side of the gas space 16 at the surface of the cathode 15 , which coalesce and collect in shape in the lower region of the cathode 15 .
  • the backup of electrolyte causes a pressure rise in the gas space 16 .
  • this pressure rise is compensated for again by the throttle 30 in that electrolyte and/or gas is recycled from the overflow vessel 26 back into the electrolyte circuit 20 .
  • the pressure differential between the two sides of the cathode 15 thus remains within the desired range between 10 and 100 hPa.
  • the OH ⁇ ions that pass through the cathode 15 do cause salt formation together with the carbon dioxide and the alkali metal cations from the electrolyte, but the pressure differential at the cathode 15 is so small that sufficient liquid is flushed through the cathode 15 and brings the salt formed into solution, permanently washes it away and transports it out of the gas space 16 into the overflow vessel 26 . A further pressure rise that would lead to crystallization of the salt formed is prevented by the throttle 30 .

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  • 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)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)
US16/312,203 2016-06-30 2017-05-18 Arrangement for the Electrolysis of Carbon Dioxide Abandoned US20190233957A1 (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE102016211824.2A DE102016211824A1 (de) 2016-06-30 2016-06-30 Anordnung für die Kohlendioxid-Elektrolyse
DE102016211824.2 2016-06-30
PCT/EP2017/061924 WO2018001636A1 (de) 2016-06-30 2017-05-18 Anordnung für die kohlendioxid-elektrolyse

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US20190233957A1 true US20190233957A1 (en) 2019-08-01

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US16/312,203 Abandoned US20190233957A1 (en) 2016-06-30 2017-05-18 Arrangement for the Electrolysis of Carbon Dioxide

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US (1) US20190233957A1 (de)
EP (1) EP3445893B1 (de)
CN (1) CN109415821A (de)
AU (1) AU2017288319B2 (de)
BR (1) BR112018075707A2 (de)
CL (1) CL2018003721A1 (de)
DE (1) DE102016211824A1 (de)
DK (1) DK3445893T3 (de)
ES (1) ES2795698T3 (de)
PL (1) PL3445893T3 (de)
WO (1) WO2018001636A1 (de)

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US10907261B2 (en) 2016-06-30 2021-02-02 Siemens Aktiengesellschaft System and method for the electrolysis of carbon dioxide
JP2022134902A (ja) * 2021-03-04 2022-09-15 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
JP2022134904A (ja) * 2021-03-04 2022-09-15 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
CN116575058A (zh) * 2023-07-13 2023-08-11 上海治臻新能源股份有限公司 多孔扩散层、水电解装置
EP4276223A1 (de) * 2022-05-09 2023-11-15 Siemens Energy Global GmbH & Co. KG Betriebsart für kohlendioxyd-elektrolyse

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DE102017213471A1 (de) * 2017-08-03 2019-02-07 Siemens Aktiengesellschaft Vorrichtung und Verfahren zur elektrochemischen Nutzung von Kohlenstoffdioxid
DE102018202344A1 (de) * 2018-02-15 2019-08-22 Siemens Aktiengesellschaft Elektrochemische Herstellung von Kohlenstoffmonoxid und/oder Synthesegas
EP3626861A1 (de) * 2018-09-18 2020-03-25 Covestro Deutschland AG Elektrolysezelle, elektrolyseur und verfahren zur reduktion von co2
DE102018222338A1 (de) * 2018-12-19 2020-06-25 Siemens Aktiengesellschaft Elektrolyseur zur Kohlenstoffdioxidreduktion
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

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US20180023203A1 (en) * 2014-12-19 2018-01-25 Repsol, S.A. Filter-press photoelectrochemical water oxidation and co2 reduction cell

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US20140131217A1 (en) * 2011-05-31 2014-05-15 Clean Chemistry, Llc Electrochemical reactor and process
US20140291163A1 (en) * 2011-07-26 2014-10-02 The Board Of Trustees Of The Leland Stanford Junior University Catalysts for low temperature electrolytic co2 reduction
US20180023203A1 (en) * 2014-12-19 2018-01-25 Repsol, S.A. Filter-press photoelectrochemical water oxidation and co2 reduction cell

Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US10907261B2 (en) 2016-06-30 2021-02-02 Siemens Aktiengesellschaft System and method for the electrolysis of carbon dioxide
JP2022134902A (ja) * 2021-03-04 2022-09-15 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
JP2022134904A (ja) * 2021-03-04 2022-09-15 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
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
JP7203875B2 (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
EP4276223A1 (de) * 2022-05-09 2023-11-15 Siemens Energy Global GmbH & Co. KG Betriebsart für kohlendioxyd-elektrolyse
WO2023220520A1 (en) * 2022-05-09 2023-11-16 Siemens Energy Global GmbH & Co. KG Carbon dioxide electrolysis operation mode
CN116575058A (zh) * 2023-07-13 2023-08-11 上海治臻新能源股份有限公司 多孔扩散层、水电解装置

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CN109415821A (zh) 2019-03-01
AU2017288319A1 (en) 2018-12-13
EP3445893B1 (de) 2020-04-01
AU2017288319B2 (en) 2019-07-25
DK3445893T3 (da) 2020-06-22
EP3445893A1 (de) 2019-02-27
WO2018001636A1 (de) 2018-01-04
CL2018003721A1 (es) 2019-02-15
BR112018075707A2 (pt) 2019-04-02
DE102016211824A1 (de) 2018-01-18
PL3445893T3 (pl) 2020-11-16
ES2795698T3 (es) 2020-11-24

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