EP4582590A1 - Elektrolyse mit nachgeschaltetem schichtungsrohr - Google Patents

Elektrolyse mit nachgeschaltetem schichtungsrohr Download PDF

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Publication number
EP4582590A1
EP4582590A1 EP24150671.6A EP24150671A EP4582590A1 EP 4582590 A1 EP4582590 A1 EP 4582590A1 EP 24150671 A EP24150671 A EP 24150671A EP 4582590 A1 EP4582590 A1 EP 4582590A1
Authority
EP
European Patent Office
Prior art keywords
pipe
flow
separator
end opening
arrangement
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.)
Pending
Application number
EP24150671.6A
Other languages
English (en)
French (fr)
Inventor
Yann Choudar
Markus NESSELBERGER
Jean-Philippe Tadiello
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.)
Air Liquide SA
LAir Liquide SA pour lEtude et lExploitation des Procedes Georges Claude
Original Assignee
Air Liquide SA
LAir Liquide SA pour lEtude et lExploitation des Procedes Georges Claude
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 Air Liquide SA, LAir Liquide SA pour lEtude et lExploitation des Procedes Georges Claude filed Critical Air Liquide SA
Priority to EP24150671.6A priority Critical patent/EP4582590A1/de
Publication of EP4582590A1 publication Critical patent/EP4582590A1/de
Pending 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
    • C25B1/00—Electrolytic production of inorganic compounds or non-metals
    • C25B1/01—Products
    • C25B1/02—Hydrogen or oxygen
    • C25B1/04—Hydrogen or oxygen by electrolysis of water
    • 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
    • C25B15/00—Operating or servicing cells
    • C25B15/08—Supplying or removing reactants or electrolytes; Regeneration of electrolytes
    • C25B15/083—Separating products
    • 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
    • C25B15/085—Removing impurities
    • 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

Definitions

  • a respective biphasic mixture of liquid electrolyte and product gas flows to the respective gas-liquid separator. It is known to recycle the respective electrolyte with a certain recycle rate and to mix them again with the electrolyte in the electrolyser.
  • Gas-liquid separators are known. Commonly, gas- liquid separators are designed as gravity separators operating according to the gravity effect, wherein the gravity separator is composed of a cylindrical vessel placed horizontally or vertically.
  • a limited efficiency of the gas-liquid separator and a high recycle rate can lead to product gas bubbles in the liquid electrolyte carry over to the liquid electrolyte in the electrolyser.
  • hydrogen bubbles in the catholyte can be carried over from the cathode side via the separator to the anode side of the electrolyser.
  • Oxygen bubbles in the anolyte can be carried over from the anode side via the separator to the cathode side of the electrolyser. This crossover can lead to higher contamination of hydrogen with oxygen and/or higher contamination of oxygen with hydrogen. Increased contamination might generate an explosive mixture after reaching a lower explosive limit, or a higher explosive limit in the case of a Hydrogen atmosphere getting additional Oxygen.
  • the first pipe end opening of the first pipe is fluidly connected to the electrolysis stack, wherein the second pipe end opening of the first pipe is fluidly connected to an inlet of the first separator.
  • a first ratio defined as a free flow area of the first pipe divided by a free flow area of the first separator is in the range of 0.002 to 0.6.
  • the arrangement can be used for electrolysis of a medium.
  • the medium is liquid, in particular water.
  • the medium may contain dissolved salts such as KOH for alkaline electrolysis or electrolysis using anion exchange membrane cells.
  • the electrolysis products are gaseous.
  • the arrangement comprises an electrolysis stack.
  • the arrangement comprises multiple electrolysis stacks.
  • the electrolysis stack comprises multiple electrolysis cells. Within the electrolysis stack the electrolysis of the medium can be performed using the electrolysis cells.
  • the arrangement is used for electrolysis in cases with a designed capacity of at least 100 kW.
  • the first gas flow can comprise the electrolysis products from the electrolysis stack.
  • a first biphasic flow is a mixture of the first gas flow and the first liquid electrolyte flow that emanates from the electrolysis stack.
  • the first gas flow can be entrapped partially in the first liquid electrolyte flow.
  • the first gas flow can be formed partially as small bubbles in the first liquid electrolyte flow.
  • the electrolysis stack can be pressurized. The first gas flow can then be formed as even smaller bubbles in the first liquid electrolyte flow.
  • the first pipe is configured to obtain a stratified flow regime of the first biphasic flow of the first liquid electrolyte flow and the first gas flow.
  • a stratified flow regime a clear spatial difference between the first liquid electrolyte flow and the first gas flow can appear.
  • the first gas flow can ascend to the top and the first liquid electrolyte flow can descend to the bottom of the first pipe due to their densities.
  • the first gas flow and the first liquid electrolyte flow can be separated by an undisturbed flat interface.
  • the first pipe is hollow.
  • no barriers or obstructions for the first gas flow and for the first liquid electrolyte flow are arranged in the first pipe.
  • the first pipe end opening of the first pipe is fluidly connected to the electrolysis stack, wherein the second pipe end opening of the first pipe is fluidly connected to the inlet of the first separator.
  • first pipe end opening of the first pipe is fluidly connected to the electrolysis stack
  • second pipe end opening of the first pipe is fluidly connected to the inlet of the first separator
  • a flow is able to flow from the electrolysis stack to the first pipe end opening of the first pipe and from the second pipe end opening of the first pipe to the first separator.
  • the first pipe can be considered a connecting piece for the first gas flow and the first liquid electrolyte flow between the electrolysis stack and the first separator.
  • the first separator is configured to separate a liquid phase and a gaseous phase of an incoming flow from each other.
  • the first separator is configured to separate the first liquid electrolyte flow and the first gas flow.
  • the first separator is a gravity separator. Two components with different densities, are separated according to their densities. Components with lighter densities with respect to the heavier densities ascend, so that a vertical separation is accomplished.
  • the first separator can be composed of a cylindrical vessel placed horizontally or vertically. It is particularly preferred that the first separator is a horizontally placed cylindrical vessel.
  • the first separator can comprise a first end and an opposite second end.
  • the first gas flow and the first liquid electrolyte flow can be injected into the first separator via the inlet of the first separator.
  • the inlet of the first separator is arranged at the first end of the first separator.
  • the inlet of the first separator is just as large as the second pipe end opening of the first pipe. The advantage of this is that turbulences are reduced and thus an unwanted mixture of first gas flow and first liquid electrolyte flow is avoided.
  • the first ratio defined as a free flow area of the first pipe divided by a free flow area of the first separator is in the range of 0.002 to 0.6.
  • the first ratio defined as a free flow area of the first pipe divided by a free flow area of the first separator is in the range of 0.0025 to 0.5625.
  • the first ratio defined as the square root of a free flow area of the first pipe divided by the square root of a free flow area of the first separator is in the range of 0.05 to 0.75.
  • a cross-sectional area of the first pipe denotes the free flow area of the first pipe. It is particularly preferred that the free flow area of the first pipe and/or the cross-sectional area of the first pipe are constant over the pipe length of the first pipe.
  • a cross-sectional area of the first separator denotes the free flow area of the first separator. It is particularly preferred that the free flow area of the first separator and/or the cross-sectional area of the first separator are constant over the length of the first separator. The "and" cases are preferred.
  • the cross-sectional area of the first pipe is rectangular and/or the cross-sectional area of the first separator is rectangular. It is particularly preferred that the cross-sectional area of the first pipe is round and/or the cross-sectional area of the first separator is round. The "and" cases are preferred.
  • the advantage of the described configuration is that a flow regime of the biphasic mixture flow in the first pipe can be adjusted.
  • a stratified flow regime can advantageously be reached.
  • reaching a stratified flow regime a clear difference between the first gas flow and the first liquid electrolyte flow in the first pipe appears.
  • reaching a stratified flow regime in the first pipe can mean that the first gas flow and the first liquid electrolyte flow in the first pipe are spatially separated due to their density.
  • the first gas flow flows on top of the liquid electrolyte flow with a flat interface between the first gas flow and the second liquid electrolyte flow.
  • a flow velocity of the first gas flow and a flow velocity of the first liquid electrolyte flow in the first pipe can be reduced. Additionally, a turbulence of the first gas flow and a turbulence of the first liquid electrolyte flow in the first pipe can be reduced.
  • the separation efficiency of the first liquid electrolyte flow and the first gas flow can be increased and additionally, explosive gas mixtures in the arrangement are avoided. This is achieved in that the first liquid electrolyte flow and the first gas flow are not only separated from each other within the first separator, but partially already within the first pipe that leads to the first separator.
  • the first pipe has a length that is at least equal to the square root of the free flow area of the first pipe.
  • the first pipe has a length that is at least four times the square root of the free flow area of the first pipe divided by the square root of pi.
  • a stratified flow regime in the first pipe can be obtained particularly well.
  • the stratified flow regime can be obtained at least towards the second pipe end opening of the first pipe.
  • the first pipe is cylindrical, wherein the first pipe end opening is opposite to the second pipe end opening. It is preferred, but not necessary that the first pipe end opening of the first pipe and the second pipe end opening of the first pipe are the same size.
  • the first pipe has an inner diameter
  • the first separator has an inner diameter
  • a second ratio defined as the inner diameter of the first pipe divided by the inner diameter of the first separator is in the range of 0.05 to 0.75.
  • the first separator is cylindrical.
  • the first pipe has a length that is at least equal to two times the inner diameter of the first pipe.
  • a stratified flow regime in the first pipe can be obtained particularly well.
  • the stratified flow regime can be obtained at least towards the second pipe end opening of the first pipe.
  • the length of the first separator can be particularly short.
  • the first separator has a gas outlet, and the first separator has an electrolyte outlet.
  • the gas outlet is arranged above the electrolyte outlet.
  • the first gas flow can be discharged from the first separator via the gas outlet.
  • the first liquid electrolyte flow can be drained from the first separator via the electrolyte outlet.
  • the first liquid flow has a higher density than the first gas flow.
  • the gas outlet and the electrolyte outlet are vertically distanced from each other as far as possible. This could mean that the gas outlet is arranged at the top of the first separator and the electrolyte outlet is arranged at the bottom of the first separator.
  • the gas outlet and the electrolyte outlet are arranged at the second end of the first separator.
  • the first gas flow and the first electrolyte flow can be separated particularly easily.
  • the first pipe is immediately connected to the inlet of the first separator.
  • an overall length of the first separator and the first pipe is particularly shortened.
  • the arrangement further comprises a second separator for separating a second gas flow and a second liquid electrolyte flow, a second pipe, which is oriented along a second horizontal axis, and which has a first pipe end opening and a second pipe end opening, wherein the first pipe end opening of the second pipe is fluidly connected to the electrolysis stack, wherein the second pipe end opening of the second pipe is fluidly connected to an inlet of the second separator, and wherein a third ratio defined as a free flow area of the second pipe divided by a free flow area of the second separator is in the range of 0.002 to 0.6.
  • the second pipe is configured to obtain a stratified flow regime of the second biphasic flow of the second liquid electrolyte flow and the second gas flow.
  • a stratified flow regime a spatial difference between the second liquid electrolyte flow and the second gas flow appears.
  • the second gas flow ascends to the top and the second liquid electrolyte flow descends to the bottom of the second pipe due to their densities.
  • the second gas flow and the second liquid electrolyte flow are separated by an undisturbed flat interface.
  • the second pipe is hollow. It is particularly preferred that no barriers or obstructions for the second gas flow and for the second liquid electrolyte flow are arranged in the second pipe.
  • the first pipe end opening of the second pipe is fluidly connected to the electrolysis stack, wherein the second pipe end opening of the second pipe is fluidly connected to the inlet of the second separator.
  • first pipe end opening of the second pipe is fluidly connected to the electrolysis stack
  • second pipe end opening of the second pipe is fluidly connected to the inlet of the second separator
  • a flow is able to flow from the electrolysis stack to the first pipe end opening of the second pipe and from the second pipe end opening of the second pipe to the second separator.
  • the second pipe can be considered a connecting piece for the second gas flow and the second liquid electrolyte flow between the electrolysis stack and the second separator.
  • the second gas flow and the second liquid electrolyte flow are injected into the second separator via the inlet of the second separator.
  • the inlet of the second separator is arranged at the first end of the second separator.
  • the inlet of the second separator is just as large as the second pipe end opening of the second pipe. The advantage of this is that turbulences are reduced and thus an unwanted mixture of second gas flow and second liquid electrolyte flow is avoided.
  • the separation efficiency of the second liquid electrolyte flow and the second gas flow can be increased and additionally, explosive gas mixtures in the arrangement are avoided. This is achieved in that the second liquid electrolyte flow and the second gas flow are not only separated from each other within the second separator, but partially already within the second pipe that leads to the second separator.
  • the first pipe end opening of the first pipe is fluidly connected to the cathode side of the electrolysis stack.
  • the first pipe end opening of the second pipe is fluidly connected to the anode side of the electrolysis stack.
  • the cathode side of the electrolysis stack is a source of the first gas flow and of the first liquid electrolyte flow.
  • the anode side of the electrolysis stack is a source of the second gas flow and of the second liquid electrolyte flow.
  • the described advantages and features of the arrangement are applicable and transferable to the method, and vice versa.
  • the arrangement is preferably set up for operation according to the method.
  • the method is preferably carried out with the arrangement.
  • the method comprises the further steps:
  • the Reynolds number of the first gas flow in the first pipe is in the range of 0.2 to 100, and the Reynolds number of the first liquid electrolyte flow in the first pipe is in the range of 2 to 100.
  • the Reynolds number of the first gas flow and the Reynolds number of the first liquid electrolyte flow can be considered separately.
  • the separate consideration of the first gas flow and the first liquid electrolyte flow can be feasible when the first liquid electrolyte flow and the first gas flow are stratified.
  • the first gas flow and/or the first liquid electrolyte flow are laminar, at least before being injected for separation into the first separator.
  • the Reynolds number of the second gas flow in the second pipe is in the range of 0.2 to 100, and the Reynolds number of the second liquid electrolyte flow in the second pipe is in the range of 2 to 100.
  • the Reynolds number of the second gas flow and the Reynolds number of the second liquid electrolyte flow can be considered separately.
  • the separate consideration of the second gas flow and the second liquid electrolyte flow can be feasible when the second liquid electrolyte flow and the second gas flow are stratified.
  • the second gas flow and/or the second liquid electrolyte flow are laminar, at least before being injected for separation in the second separator.
  • the first electrolyte flow in the first pipe comprises water, and the first gas flow in the first pipe comprises an electrolysis product.
  • the first gas flow in the first pipe can comprise hydrogen.
  • the second electrolyte flow in the second pipe comprises water, and the second gas flow in the second pipe comprises an electrolysis product.
  • the second gas flow in the second pipe can comprise oxygen.
  • the recycled first liquid electrolyte flow volume of the first separator is in the range between 0.05 and 50 m 3 /h and/or the recycled second liquid electrolyte flow volume of the second separator is in the range between 0.05 and 50 m 3 /h.
  • the entire recycled liquid electrolyte flow volume is in the range between 0.1 and 100 m 3 /h, wherein the entire recycle liquid electrolyte flow comprises the recycled first liquid electrolyte flow volume of the first separator and the recycled second liquid electrolyte flow volume of the second separator.
  • Figure 1 schematically shows an arrangement 1 for electrolysis, which comprises:
  • the first pipe end opening 10.1 of the first pipe 5.1 is fluidly connected to the electrolysis stack 2, wherein the second pipe end opening 11.1 of the first pipe 5.1 is fluidly connected to an inlet 13.1 of the first separator 6.1.
  • a first ratio R 1 defined as a free flow area A P1 of the first pipe 5.1 divided by a free flow area A S1 of the first separator 6.1 is in the range of 0.002 to 0.6.
  • the first pipe 5.1 has a length L P1 that is at least equal to the square root of the free flow area A P1 of the first pipe 5.1.
  • the first separator 6.1 has a gas outlet 14.1 and the first separator 6.1 has an electrolyte outlet 15.1, wherein the gas outlet 14.1 is arranged above the electrolyte outlet 15.1.
  • the first pipe 5.1 is immediately connected to the inlet 13.1 of the first separator 6.1.
  • the arrangement 1 further comprises:
  • the first pipe end opening 10.2 of the second pipe 5.2 is fluidly connected to the electrolysis stack 2, wherein the second pipe end opening 11.2 of the second pipe 5.2 is fluidly connected to an inlet 13.2 of the second separator 6.2.
  • a third ratio R 3 defined as a free flow area A P2 of the second pipe 5.2 divided by a free flow area A S2 of the second separator 6.2 is in the range of 0.002 to 0.6.
  • the second pipe 5.2 has a length L P2 that is at least equal to the square root of the free flow area A P2 of the second pipe 5.2.
  • the second separator 6.2 has a gas outlet 14.2 and the second separator 6.2 has an electrolyte outlet 15.2, wherein the gas outlet 14.2 is arranged above the electrolyte outlet 15.2.
  • the second pipe 5.2 is immediately connected to the inlet 13.2 of the second separator 6.2.
  • the first electrolyte flow 9.1 in the first pipe 5.1 comprises water, and the first gas flow 8.1 in the first pipe 5.1 comprises hydrogen as an electrolysis product.
  • the second electrolyte flow 9.2 in the second pipe 5.2 comprises water, and the second gas flow 8.2 in the second pipe 5.2 comprises oxygen as an electrolysis product.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Inorganic Chemistry (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
EP24150671.6A 2024-01-08 2024-01-08 Elektrolyse mit nachgeschaltetem schichtungsrohr Pending EP4582590A1 (de)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP24150671.6A EP4582590A1 (de) 2024-01-08 2024-01-08 Elektrolyse mit nachgeschaltetem schichtungsrohr

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
EP24150671.6A EP4582590A1 (de) 2024-01-08 2024-01-08 Elektrolyse mit nachgeschaltetem schichtungsrohr

Publications (1)

Publication Number Publication Date
EP4582590A1 true EP4582590A1 (de) 2025-07-09

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Family Applications (1)

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EP24150671.6A Pending EP4582590A1 (de) 2024-01-08 2024-01-08 Elektrolyse mit nachgeschaltetem schichtungsrohr

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Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013063374A (ja) * 2011-09-15 2013-04-11 Vantec:Kk 気液分離器及び気体発生装置
CN114990632A (zh) * 2022-05-06 2022-09-02 华东理工大学 设置倾斜板强化气液分离器微细气泡脱离的装置和方法
WO2023232988A1 (en) * 2022-06-03 2023-12-07 Universiteit Antwerpen Electrolysis reactor

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2013063374A (ja) * 2011-09-15 2013-04-11 Vantec:Kk 気液分離器及び気体発生装置
CN114990632A (zh) * 2022-05-06 2022-09-02 华东理工大学 设置倾斜板强化气液分离器微细气泡脱离的装置和方法
WO2023232988A1 (en) * 2022-06-03 2023-12-07 Universiteit Antwerpen Electrolysis reactor

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