EP3445893B1 - Anordnung für die kohlendioxid-elektrolyse - Google Patents
Anordnung für die kohlendioxid-elektrolyse Download PDFInfo
- Publication number
- EP3445893B1 EP3445893B1 EP17724054.6A EP17724054A EP3445893B1 EP 3445893 B1 EP3445893 B1 EP 3445893B1 EP 17724054 A EP17724054 A EP 17724054A EP 3445893 B1 EP3445893 B1 EP 3445893B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- arrangement
- gas
- cathode
- space
- electrolyte
- 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.)
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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
- 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
-
- 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
- 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
- the invention relates to an arrangement for carbon dioxide electrolysis according to the preamble of claim 1.
- CO2 is a strongly bound molecule and can therefore be reduced to usable products only with difficulty.
- CO2 is converted to carbohydrates by photosynthesis. This complex process is very difficult to replicate on an industrial scale.
- the electrochemical reduction of CO2 is currently a technically feasible way.
- the carbon dioxide is converted into an energetically higher-quality product such as CO, CH4, C2H4 or C1-C4 alcohols by supplying electrical energy.
- the electrical energy in turn comes preferably from renewable energy sources such as wind power or photovoltaics.
- Metals are generally used as catalysts for the electrolysis of CO2.
- the type of metal influences the products of electrolysis.
- CO2 is reduced almost exclusively to CO on Ag, Au, Zn, and with restrictions on Pd, Ga, whereas a large number of hydrocarbons can be observed as reduction products on copper.
- a gas diffusion electrode (GDE) can be used as a cathode, similar to chlorine-alkali electrolysis, to establish a three-phase boundary between the liquid electrolyte, the gaseous CO2 and the solid silver particles.
- GDE gas diffusion electrode
- An electrolysis cell as is also known from fuel cell technology, is used with two electrolyte chambers, the electrolyte chambers being separated by an ion exchange membrane.
- the working electrode is a porous gas diffusion electrode. It comprises a metal mesh on which a mixture of PTFE, activated carbon, a catalyst and other components is applied. It comprises a pore system into which the reactants penetrate and react at the three-phase interfaces.
- the counter electrode is a sheet loaded 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 CO2, which is pressed through with excess pressure by the GDE (so-called convective mode of operation).
- the GDE can contain various metals and metal compounds that have a catalytic effect on the process.
- the functionality of a GDE is, for example, from the EP 297377 A2 , of the EP 2444526 A2 and the EP 2410079 A2 known.
- the resulting product 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. Because of of the operating conditions, the salts in and on the GDE crystallize from the gas side.
- the arrangement according to the invention for carbon dioxide electrolysis comprises an electrolytic cell with an anode and a cathode, the anode and cathode being connected to a voltage supply, the cathode being designed as a gas diffusion electrode to which a gas space is attached on a first side and a gas space on a second side Connects to the cathode compartment, an electrolyte circuit connected to the electrolytic cell, for supplying an anode compartment and the cathode compartment with a liquid electrolyte, and a gas supply for supplying gas containing carbon dioxide into the gas compartment.
- the gas space has an outlet for electrolyte, carbon dioxide and product gases from the electrolysis and the outlet is connected to the electrolyte circuit via a throttle, the throttle being designed, a definable pressure difference between the gas space and cathode space when a mixture of product gases and liquid electrolyte flows through to effect.
- the structure of an electrolysis cell 11 shown schematically in FIG. 1 is typically suitable for carrying out a carbon dioxide electrolysis.
- the embodiment of the electrolytic cell 11 comprises at least one anode 13 with adjacent anode space 12 and a cathode 15 and an adjacent cathode space 14.
- Anode space 12 and cathode space 14 are separated from one another by a membrane 21.
- the membrane 21 is typically made of a PTFE-based material.
- a construction without a membrane 21 is also conceivable, in which case a pH compensation goes beyond 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 electrolytic cell 11 shown is equipped with an electrolyte inlet.
- the anode space 12 shown includes an outlet for electrolyte and, for example, oxygen O 2 or another gaseous by-product, which is formed on the anode 13 during carbon dioxide electrolysis.
- the cathode compartment 14 also has at least one product and electrolyte outlet.
- the total electrolysis product can be composed of a large number of electrolysis products.
- the electrolysis cell 11 is also designed in a three-chamber structure in which the carbon dioxide CO 2 flows into the cathode space 14 via the cathode 15 designed as a gas diffusion electrode.
- Gas diffusion electrodes make it possible to bring a solid catalyst, a liquid electrolyte and a gaseous electrolysis adduct into contact with one another.
- the catalyst can be porous and take over the electrode function, or a porous electrode takes over the catalyst function.
- the pore system of the electrode is designed such that the liquid and the gaseous phase can penetrate the pore system equally and can be present in it or on its electrically accessible surface at the same time.
- An example of a gas diffusion electrode is an oxygen depletion electrode used in chlor-alkali electrolysis.
- the cathode 15 in this example comprises a metal network to which a mixture of PTFE, activated carbon and a catalyst is applied.
- the electrolytic cell 11 comprises a carbon dioxide inlet 24 in the gas space 16. The carbon dioxide reaches the cathode 15 in the gas space 16 and can penetrate there into the porous structure of the cathode 15 and thus react.
- the arrangement 10 further comprises an electrolyte circuit 20, via which the anode compartment 12 and the cathode compartment 14 are supplied with a liquid electrolyte, for example K2SO4, KHCO3, KOH, Cs2SO4, and the electrolyte is returned to a reservoir 19.
- a liquid electrolyte for example K2SO4, KHCO3, KOH, Cs2SO4, and the electrolyte is returned to a reservoir 19.
- the electrolyte is circulated in the electrolyte circuit 20 by an electrolyte pump 18.
- the gas space 16 comprises an outlet 25 which is arranged in the floor area.
- the outlet 25 is designed as an opening with a sufficient cross-section so that both electrolyte that passes through the cathode 15 and carbon dioxide and product gases can get into the connected pipe through the outlet.
- the outlet 25 leads to an overflow vessel 26.
- the liquid electrolyte is collected in the overflow vessel 26 and collects. Carbon dioxide and product gases coming from the gas space 16 are separated from the electrolyte and collect above it.
- a further pipe 28 leads to a pump 27, in this exemplary embodiment a diaphragm pump, and further to the gas supply 17.
- the pump 27 can also be a piston, stroke, extruder or gear pump.
- the carbon dioxide and existing product gases are led back from the overflow vessel 26 into the gas supply and thus the gas is partly circulated.
- the volume flow of the pump 27 is significantly higher than the volume flow of new carbon dioxide.
- Starting gas, which is not consumed, is advantageously guided past the cathode 15 again and has the opportunity to be reduced one more time or several times. Some of the product gases are also circulated. By repeatedly passing the carbon dioxide past the cathode 15, the efficiency of the conversion is increased.
- the overflow vessel 26 There is a further connection from the overflow vessel 26 which leads back to the electrolyte circuit 20.
- This connection begins with an outlet 29, which is arranged on a side wall of the overflow vessel 26, preferably near the bottom, but not in the bottom.
- the outlet 29 is connected to a throttle 30, which is designed as a vertical tube piece with a length of 90 cm, for example.
- the diameter of the pipe section is significantly larger than that of the feed lines to the throttle 30.
- the feed line has, for example, an inner diameter of 4 mm, the pipe section has an inner diameter of 20 mm.
- the choke 30 is on the output side, i.e. connected to the electrolyte circuit 20 at the upper end of the pipe section.
- the throttle 30 produces and maintains a pressure difference between the electrolyte circuit 20 connected at the top and thus also the cathode chamber 14 on the one hand and the overflow vessel 26 and the gas chamber 16 on the other hand.
- This pressure difference is between 10 and 100 hPa (mbar), ie the gas space 16 remains at only a slight overpressure in relation to the cathode space 14.
- the throttle 30 produces the pressure difference regardless of whether a liquid or gaseous medium is flowing through or a mixture of them.
- the differential pressure is set as a function of the height of the pipe section due to the hydrostatic pressure. Will the pipe piece rotatably mounted, the differential pressure of the throttle 30 can be continuously reduced down to almost zero in a horizontal position.
- the accumulating electrolyte thereby causes an increase in pressure in the gas space 16.
- this pressure increase is compensated for again by the throttle 30, in that electrolyte and / or gas is returned from the overflow vessel 26 to the electrolyte circuit 20.
- the pressure difference between the two sides of the cathode 15 thus remains in the desired range between 10 and 100 hPa.
- the OH - ions passing through the cathode 15 cause salt formation together with the carbon dioxide and the alkali metal ions from the electrolyte, but the differential pressure at the cathode 15 is so low that sufficient liquid is flushed through the cathode 15 and the salt formed in Bring solution, wash off permanently and transported from the gas space 16 into the overflow vessel 26. A further increase in pressure, which 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)
- Inorganic Chemistry (AREA)
- Automation & Control Theory (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
- Electrodes For Compound Or Non-Metal Manufacture (AREA)
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
PL17724054T PL3445893T3 (pl) | 2016-06-30 | 2017-05-18 | Układ do elektrolizy dwutlenku węgla |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE102016211824.2A DE102016211824A1 (de) | 2016-06-30 | 2016-06-30 | Anordnung für die Kohlendioxid-Elektrolyse |
PCT/EP2017/061924 WO2018001636A1 (de) | 2016-06-30 | 2017-05-18 | Anordnung für die kohlendioxid-elektrolyse |
Publications (2)
Publication Number | Publication Date |
---|---|
EP3445893A1 EP3445893A1 (de) | 2019-02-27 |
EP3445893B1 true EP3445893B1 (de) | 2020-04-01 |
Family
ID=58709995
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP17724054.6A Active EP3445893B1 (de) | 2016-06-30 | 2017-05-18 | Anordnung für die kohlendioxid-elektrolyse |
Country Status (11)
Country | Link |
---|---|
US (1) | US20190233957A1 (da) |
EP (1) | EP3445893B1 (da) |
CN (1) | CN109415821A (da) |
AU (1) | AU2017288319B2 (da) |
BR (1) | BR112018075707A2 (da) |
CL (1) | CL2018003721A1 (da) |
DE (1) | DE102016211824A1 (da) |
DK (1) | DK3445893T3 (da) |
ES (1) | ES2795698T3 (da) |
PL (1) | PL3445893T3 (da) |
WO (1) | WO2018001636A1 (da) |
Families Citing this family (10)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE102016211822A1 (de) | 2016-06-30 | 2018-01-04 | Siemens Aktiengesellschaft | Anordnung und Verfahren für die Kohlendioxid-Elektrolyse |
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 |
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 |
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 |
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 |
EP4276223A1 (en) * | 2022-05-09 | 2023-11-15 | Siemens Energy Global GmbH & Co. KG | Carbon dioxide electrolysis operation mode |
CN116575058B (zh) * | 2023-07-13 | 2023-10-31 | 上海治臻新能源股份有限公司 | 多孔扩散层、水电解装置 |
Family Cites Families (15)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US3679565A (en) * | 1971-07-27 | 1972-07-25 | Scm Corp | Process for electrolytic treatment of liquors using pressure cell with porous electrode means |
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 |
CN101649464A (zh) * | 2008-08-11 | 2010-02-17 | 浙江工业大学 | 二氧化碳分解制氧器 |
DE102010031571A1 (de) | 2010-07-20 | 2012-01-26 | Bayer Materialscience Ag | Sauerstoffverzehrelektrode |
WO2012040503A2 (en) * | 2010-09-24 | 2012-03-29 | Det Norske Veritas As | Method and apparatus for the electrochemical reduction of carbon dioxide |
DE102010042729A1 (de) | 2010-10-21 | 2012-04-26 | Bayer Materialscience Aktiengesellschaft | Sauerstoffverzehrkathode und Verfahren zu ihrer Herstellung |
CN102181876B (zh) * | 2011-03-30 | 2012-12-19 | 昆明理工大学 | 一种电化学催化还原二氧化碳制备一氧化碳的方法与装置 |
WO2012164913A1 (ja) * | 2011-05-31 | 2012-12-06 | パナソニック株式会社 | 二酸化炭素富化デバイス |
WO2012166997A2 (en) * | 2011-05-31 | 2012-12-06 | Clean Chemistry, Llc | Electrochemical reactor and process |
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 |
WO2013178803A1 (de) * | 2012-05-31 | 2013-12-05 | Hettich Holding Gmbh & Co. Ohg | Verfahren und vorrichtung zur elektrolytischen synthese von methanol und/oder methan |
DE102013226357A1 (de) * | 2013-12-18 | 2015-06-18 | Siemens Aktiengesellschaft | Pulsierende Elektrolytzufuhr in den Reaktionsraum einer Elektrolysezelle mit gasentwickelnden Elektroden |
CN103741164B (zh) * | 2014-01-03 | 2016-07-06 | 南开大学 | 一种电化学还原co2制甲酸的气体扩散电极的制备方法 |
PT3234224T (pt) * | 2014-12-19 | 2018-10-18 | Repsol Sa | Células fotoeletroquímicas filtro-pressão para a redução do co2 e oxidação da água |
-
2016
- 2016-06-30 DE DE102016211824.2A patent/DE102016211824A1/de not_active Withdrawn
-
2017
- 2017-05-18 ES ES17724054T patent/ES2795698T3/es active Active
- 2017-05-18 CN CN201780040306.1A patent/CN109415821A/zh active Pending
- 2017-05-18 PL PL17724054T patent/PL3445893T3/pl unknown
- 2017-05-18 WO PCT/EP2017/061924 patent/WO2018001636A1/de unknown
- 2017-05-18 EP EP17724054.6A patent/EP3445893B1/de active Active
- 2017-05-18 DK DK17724054.6T patent/DK3445893T3/da active
- 2017-05-18 US US16/312,203 patent/US20190233957A1/en not_active Abandoned
- 2017-05-18 AU AU2017288319A patent/AU2017288319B2/en not_active Ceased
- 2017-05-18 BR BR112018075707-1A patent/BR112018075707A2/pt not_active IP Right Cessation
-
2018
- 2018-12-20 CL CL2018003721A patent/CL2018003721A1/es unknown
Non-Patent Citations (1)
Title |
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None * |
Also Published As
Publication number | Publication date |
---|---|
ES2795698T3 (es) | 2020-11-24 |
AU2017288319B2 (en) | 2019-07-25 |
CL2018003721A1 (es) | 2019-02-15 |
DK3445893T3 (da) | 2020-06-22 |
AU2017288319A1 (en) | 2018-12-13 |
US20190233957A1 (en) | 2019-08-01 |
BR112018075707A2 (pt) | 2019-04-02 |
WO2018001636A1 (de) | 2018-01-04 |
EP3445893A1 (de) | 2019-02-27 |
PL3445893T3 (pl) | 2020-11-16 |
DE102016211824A1 (de) | 2018-01-18 |
CN109415821A (zh) | 2019-03-01 |
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