EP1651799B1 - Cellule electrochimique - Google Patents

Cellule electrochimique Download PDF

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Publication number
EP1651799B1
EP1651799B1 EP04740955.2A EP04740955A EP1651799B1 EP 1651799 B1 EP1651799 B1 EP 1651799B1 EP 04740955 A EP04740955 A EP 04740955A EP 1651799 B1 EP1651799 B1 EP 1651799B1
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EP
European Patent Office
Prior art keywords
gas
gap
electrolyte
cell
diffusion electrode
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.)
Expired - Lifetime
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EP04740955.2A
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German (de)
English (en)
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EP1651799A1 (fr
Inventor
Andreas Bulan
Michael Grossholz
Volker Michele
Hans-Joachim Brockhaus
Hans-Dieter Pinter
Fritz Gestermann
Rainer Weber
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Bayer Intellectual Property GmbH
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Bayer Intellectual Property GmbH
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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
    • 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 electrochemical cell, at least consisting of an anode half-cell with an anode, a cathode half-cell with a cathode and an ion exchange membrane arranged between anode half-cell and cathode half-cell, wherein the anode and / or the cathode is a gas diffusion electrode.
  • the invention further relates to a process for the electrolysis of an aqueous solution of alkali chloride.
  • WO-A 01/57290 An electrolytic cell with a gas diffusion electrode is known in which a porous layer is provided in the gap between the gas diffusion electrode and the ion exchange membrane. The electrolyte flows from top to bottom over the porous layer under the action of gravity through the gap.
  • the porous layer according to WO-A 01/57290 can be made of foams, wire nets or the like. consist.
  • an electrolytic cell with gas diffusion electrode for the electrolysis of a sodium chloride solution in which a layer of a hydrophilic material is in the gap between the gas diffusion electrode and the ion exchange membrane.
  • the layer of hydrophilic material preferably has a porous structure containing a corrosion-resistant metal or resin.
  • a porous structure for example, nets, fabrics or foams can be used.
  • Sodium hydroxide, the electrolyte flows down the layer of hydrophilic material down to the bottom of the electrolytic cell under gravity.
  • EP-A 1 033 419 an electrolytic cell with gas diffusion electrode as a cathode for the electrolysis of a sodium chloride solution known.
  • a hydrophilic porous material through which the electrolyte flows.
  • porous material metals metal oxides or organic materials are considered, provided they are corrosion resistant.
  • a disadvantage of the electrolytic cells with gas diffusion electrode known from the prior art is that the gap between gas diffusion electrode and ion exchange membrane can not be completely filled with electrolyte due to the porous material. This creates areas in the gap where gas is located and accumulates. No electrical current can flow in these areas. Current flows exclusively through electrolyte-filled areas in the gap, so that locally generates a higher current density, which has a higher electrolysis voltage result. Gathers the gas on the ion exchange membrane, this may be damaged due to the lack of electrolyte. Porous layers also have the disadvantage that gas which has once entered the porous structure, from this difficult to get out again. Within the porous layer, the gas can accumulate, whereby the above-mentioned disadvantages arise. Gas from the gas space can also pass through the gas diffusion electrode from the gas space into the gap under operating conditions.
  • the object of the present invention is therefore to provide an electrolytic cell which avoids the disadvantages of the prior art.
  • the invention relates to an electrochemical cell, at least consisting of an anode half-cell with an anode, a cathode half-cell with a cathode and an ion exchange membrane arranged between anode half-cell and cathode half-cell, wherein the anode and / or the cathode is a gas diffusion electrode and between the gas diffusion electrode and the ion exchange membrane Gap is arranged and the half-cell with gas diffusion electrode has an electrolyte inlet and an electrolyte outlet and a gas inlet and a gas outlet, characterized in that the electrolyte inlet is sealed to the gap according to claim 1.
  • the electrolyte flows in the gap between gas diffusion electrode and ion exchange membrane from top to bottom through the half cell.
  • the gap is completely filled with electrolyte.
  • the remaining space of the half cell, the gas space is filled with gas, which is supplied by the gas inlet and discharged through the gas outlet.
  • the electrolyte feed is tightly connected to the gap. This prevents gas from entering the gap via the electrolyte feed into the gap. Due to the tight connection between the electrolyte inlet and the gap, the electrolyte can be conveyed through the gap by means of a pump, so that the electrolyte flow does not flow in free fall in the gap along the gas diffusion electrode. With the help of the pump, the volume flow of the electrolyte flowing through the gap can be adjusted. The volume flow is preferably adjusted so that the flow velocity of the electrolyte is lower than in free fall.
  • flow guide structures are provided in the gap.
  • the flow guiding structures also prevent a free fall of the electrolyte in the gap, so that the flow velocity is reduced compared to the free fall. At the same time, however, the electrolyte must not accumulate in the gap due to the Strömungsleit Modellen.
  • the flow guide structures are chosen so that the pressure loss the hydrostatic fluid column in the gap is compensated. If flow guide structures are provided, they can completely take over the function of the pump, namely the reduction of the flow velocity in the gap, so that no pump is necessary. However, it is also possible to use a pump in combination with flow guide structures.
  • the Strömungsleit Jardin consist of thin plates, films or the like., Which have openings for the passage of the electrolyte. They are transversal, i. perpendicular or oblique, arranged to the flow direction of the electrolyte in the gap.
  • the plate-shaped Strömungsleit Modellen are preferably inclined relative to the horizontal, wherein they are inclined either only in one axis or in both axes. If the flow guide structures are arranged obliquely to the flow direction, they can be inclined both in the direction of the ion exchange membrane and in the direction of the gas diffusion electrode.
  • the inclination in the direction of the gas diffusion electrode or the ion exchange membrane corresponds to an inclination about an axis which is parallel to the gas diffusion electrode or ion exchange membrane and horizontal.
  • the flow guiding structures may be inclined across the width of the electrochemical cell. This corresponds to an inclination about an axis which is perpendicular to the gas diffusion electrode or ion exchange membrane. This inclination can be 0 to 45 °, preferably 3 to 15 °.
  • the gas diffusion electrode Since, during operation of the electrochemical cell, even small amounts of gas are always released from the space behind the gas diffusion electrode, i. the ion exchange membrane from the facing space of the half-cell, passes through the gas diffusion electrode in the flowed through with electrolyte gap, it must be ensured that the gas is discharged from the gap. As the content of gas in the electrolyte increases, the resistance of the electrolyte increases. If flow guide structures are present in the gap, the gas can either escape upwards through openings in the flow guide structures or it can be carried along by the flow of electrolyte downwards. The inclination of the flow guide structures promotes in particular the discharge of the gas bubbles upwards.
  • the flow guide structures are further arranged to contact the gas diffusion electrode on the one hand and the ion exchange membrane on the other hand.
  • the electrolyte passes only through the openings of the conductive structures.
  • the flow guide structures may be fixedly or detachably connected to the gas diffusion electrode and the ion exchange membrane.
  • the flow guide structures are preferably clamped between the gas diffusion electrode and the ion exchange membrane.
  • the Strömungsleit Jardin are attached to a in the gap substantially vertically, that is substantially parallel to the gas diffusion electrode and the ion exchange membrane, arranged holding structure.
  • the holding structure extends, for example, in the middle of the gap, so that the flow guide structures protrude on the one hand in the direction of the ion exchange membrane, on the other hand in the direction of the gas diffusion electrode.
  • the support structure consists for example of a thin plastic rod whose diameter is smaller than the gap width between gas diffusion electrode and ion exchange membrane.
  • the number of support structures, for example in the form of plastic rods, over the length of the gas diffusion electrode, and thus the Strömungsleitpatenteden, is dependent on the material thickness of the Strömungsleit fabricaten, since the plastic rods, the stability, eg when assembling the electrolyzer, effect.
  • the flow guide structures can be flat. In order to facilitate trapping of the flow guide structures between the gas diffusion electrode and the ion exchange membrane, the flow guide structures can have, for example, a Z, L, T, double T or trapezoidal profile.
  • the flow guide structures can also be arbitrarily angled or curved. Preferably, they consist of an elastic plate which is wider than the width of the gap. When pinched between the gas diffusion electrode and the ion exchange membrane and under the influence of the flow of electrolyte in the gap, the elastic plates bend downwards. The flow guide structures are then curved downwards. However, it is also possible to use upwardly curved flow guide structures. Curved Strömungsleit Jardin are advantageous because they compensate for manufacturing tolerances of the electrochemical cell, which manifest themselves, for example, in the width of the gap.
  • the opening in the flow guide structures may have any shape, e.g. round or angular.
  • the openings in superimposed or mutually arranged Strömungsleit Weg can either be superimposed or with each other, i. the openings coincide.
  • the electrolyte flow in this case runs essentially perpendicularly through the gap. However, they can also be offset from each other, so that the electrolyte flow is not rectilinear, but for example, zigzag or meandering flows through the gap. This reduces the formation of dead zones.
  • the flow guide structures can be made of a non-prone material, in particular of a non-prone metal or plastic.
  • a non-prone metal or plastic For example, nickel or PTFE can be used as the material.
  • the number of Strömungsleit Jardin and the number and the cross-sectional area of the openings are chosen so that the flow velocity of the electrolyte is lower than in free fall.
  • a height of the electrolyzer of e.g. 1.3 m and an amount of electrolyte of e.g. 180 1 / h can e.g. 26 flow guide structures with 64 openings can be used.
  • the openings have e.g. a diameter of 1 mm.
  • 6 flow guide structures with 127 openings of 0.5 mm diameter could be used.
  • a corresponding pressure compensation can be achieved via the diameter and the number of openings as well as the number of flow guiding structures.
  • the electrolyte flowing downwards in the gap must not build up on the flow guide structures. Therefore, it must be ensured that the sum of the cross-sectional areas of all openings of a flow-guiding structure is the same for all flow-guiding structures. This can be done by varying the number of openings or the cross-sectional area.
  • the preferred volume flow of the electrolyte in the gap is 100 to 300 l / h.
  • the volume flow is preferably a maximum of 500 l / h.
  • the flow rate is preferably at most 1 cm / s.
  • the advantage of flow guide structures over the porous layers known from the prior art is the improved removal of gas bubbles entering the gap through the gas diffusion electrode. Furthermore, the electrolyte is pumped through the gap between gas diffusion electrode and ion exchange membrane, whereby this gap is completely filled with electrolyte. Porous structures, which the electrolyte according to the prior art undergoes in free fall, are usually not completely filled with electrolyte, which is manifested by a higher electrolysis voltage.
  • the electrochemical cell according to the invention can be used for different electrolysis processes, in which at least one electrode is a gas diffusion electrode.
  • the gas diffusion electrode acts as a cathode, particularly preferably as an oxygen-consuming cathode, wherein the gas supplied to the electrochemical cell is an oxygen-containing gas, for example air, oxygen-enriched air or oxygen itself.
  • the cell according to the invention is preferably used for the electrolysis of an aqueous solution of an alkali halide, in particular of sodium chloride.
  • the gas diffusion electrode is constructed, for example, as follows:
  • the gas diffusion electrode consists at least of an electrically conductive carrier and an electrochemically active coating.
  • the electrically conductive carrier is preferably a mesh, woven, braided, knitted, nonwoven or foam of metal, in particular of nickel, silver or silver-plated nickel.
  • the electrochemically active coating preferably consists of at least one catalyst, e.g. Silver (I) oxide, and a binder, e.g. Polytetrafluoroethylene (PTFE).
  • the electrochemically active coating may be composed of one or more layers.
  • a gas diffusion layer for example of a mixture of carbon and polytetrafluoroethylene, can be provided, which is applied to the support.
  • electrodes of titanium may be used, which are e.g. coated with ruthenium-iridium oxides or ruthenium oxide.
  • ion exchange membrane a commercially available membrane, e.g. DuPont, Nafion NX2010.
  • the electrolysis cell according to the invention which is suitable for the electrolysis of an aqueous sodium chloride solution, has a gap between gas diffusion electrode and ion exchange membrane with a width of the order of 3 mm.
  • the flow guide structures are preferably made of thin sheets of PTFE or PVDF and have a thickness of 0.1 to 0.5 mm
  • the electrolyte inlet is a channel, for example a tube, which extends over the entire length of the gas diffusion electrode.
  • the electrolyte can be fed uniformly over the entire length from above into the gap between the gas diffusion electrode and the ion exchange membrane.
  • the feed can also take place only in one region, for example in the upper region of one of the two ends of the gas diffusion electrode.
  • the aid of the flow guide structures which are inclined in an axis perpendicular to the gas diffusion electrode or to the ion exchange membrane, a uniform distribution of the electrolyte over the entire length of the gap can be effected.
  • Another object of the invention is a method for the electrolysis of an aqueous alkali halide solution in an electrochemical cell, at least consisting of an anode half-cell with an anode, a cathode half-cell with a cathode and an arranged between the anode half-cell and cathode half-cell ion exchange membrane, wherein, the anode and / or the cathode is a gas diffusion electrode and a gap is arranged between the gas diffusion electrode and the ion exchange membrane and the half cell with a gas diffusion electrode has an electrolyte inlet and an electrolyte outlet and a gas inlet and a gas outlet, characterized in that the electrolyte by means of a pump in the gap from above flows down, the gap is completely filled with electrolyte.
  • an electrochemical cell 1 according to the invention is shown, which is constructed from an anode half cell 2 with an anode 21 and a cathode half cell 3 with a gas diffusion electrode 31 as a cathode.
  • the two half-cells 2, 3 are separated from each other by an ion exchange membrane 4.
  • the gas diffusion electrode 31 is separated from the ion exchange membrane 4 by a gap 32.
  • Seals 39 seal the half-cell 3 to the outside.
  • the cathode half-cell 3 has an electrolyte inlet 33 and an electrolyte outlet 34 as well as a gas inlet 35 and a gas outlet 36.
  • the electrolyte inlet 33 is tightly connected to the gap 32.
  • the electrolyte is supplied via the electrolyte inlet 33 of the half-cell 3 and flows in the gap 32 down before it is discharged via the electrolyte effluent 34 from the half-cell 3.
  • the gap 32 is completely filled with electrolyte during operation of the electrolysis cell 1.
  • Gas is supplied via the gas inlet 35 to the gas space 37 of the half-cell 3, flows upwards in the gas space 37 and is discharged from the half-cell 3 via the gas outlet 36.
  • the tight connection of the electrolyte inlet 33 with the gap 32 makes it possible to promote the electrolyte by means of a pump through the gap 32 and so a desired volume flow or a desired flow rate of the electrolyte in gap 32.
  • the tight connection must prevent gas from flowing from the gas space 37 into the gap 32.
  • the electrolyte feed 33 is completely filled.
  • the compensation opening 38 is to be dimensioned such that a very small volume flow of the electrolyte flows through the opening 38 into the gas space 37.
  • the volume flow through the opening 38 in the back space is less than 5% of the total volume flow.
  • the compensation opening 38 allows gas to escape, which enters the gap 32 in small quantities from the gas space 37 through the gas diffusion electrode 31 during operation of the electrolytic cell 1 and rises in the form of gas bubbles. In this way, the gas can pass from the gap 32 via the compensation opening 38 in the electrolyte inlet 33 into the gas space 37.
  • the electrolysis cell 1 in FIG. 2 in addition to the tight connection of the electrolyte inlet 33 with the gap 32 Strömungsleit Quilt Quilt 51, 52, 53, 54 in the gap 32.
  • the flow guide structures 51, 52, 53, 54 reduce the flow rate of the electrolyte in the gap 32 with respect to the flow rate that the electrolyte would assume in free fall.
  • the flow guide structures 51, 52, 53, 54 consist of thin plates with openings 56, which allow a passage of the electrolyte. They are clamped in the illustrated embodiments between the ion exchange membrane 4 and the gas diffusion electrode 31.
  • the flow guide structures 51 are arranged in the gap 32 substantially horizontally, ie transversely to the flow direction of the electrolyte.
  • the flow guide structures 53 can be arranged obliquely, ie inclined at an angle to the flow direction, for example in the direction of the ion exchange membrane 4.
  • the flow guide structures 53 are V-shaped.
  • the flow guide structures 54 are curved downwards.

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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)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)

Claims (5)

  1. Cellule électrochimique (1) constituée au moins d'une demi-cellule anodique (2) dotée d'une anode (21), d'une demi-cellule cathodique (3) dotée d'une cathode (31) et d'une membrane (4) échangeuse d'ions disposée entre la demi-cellule anodique (2) et la demi-cellule cathodique (3),
    l'anode (21) et/ou la cathode (31) étant des électrodes à diffusion de gaz et un interstice (32) étant disposé entre l'électrode (31) à diffusion de gaz et la membrane (4) échangeuse d'ions,
    les demi-cellules (2, 3) dotées d'une électrode (31) à diffusion de gaz présentant une amenée d'électrolyte (33) et une sortie d'électrolyte (34) ainsi qu'une entrée de gaz (35) et qu'une sortie de gaz (36),
    caractérisée en ce que
    l'amenée d'électrolyte (33) est raccordée de manière étanche à l'interstice (32) de manière obtenir un espace de gaz (37) en aval de l'électrode (31) à diffusion de gaz et
    en ce que l'espace de gaz (37) présente une entrée de gaz (35) et une sortie de gaz (36).
  2. Cellule électrochimique selon la revendication 1, caractérisée en ce que des structures (51; 52; 53; 54) de guidage d'écoulement sont disposées dans l'interstice (32).
  3. Cellule électrochimique selon l'une des revendications 1 ou 2, caractérisée en ce que les structures (51; 52; 53; 54) de guidage d'écoulement sont serrées entre l'électrode (31) à diffusion de gaz et la membrane (4) échangeuse d'ions.
  4. Cellule électrochimique selon l'une des revendications 1 à 3, caractérisée en ce que les structures (51; 52; 53; 54) de guidage d'écoulement sont inclinées par rapport à l'horizontale.
  5. Procédé d'électrolyse d'une solution aqueuse d'halogénure de métal alcalin dans une cellule électrochimique (1) constituée au moins d'une demi-cellule anodique (2) dotée d'une anode (21), d'une demi-cellule cathodique (3) dotée d'une cathode (31) et d'une membrane (4) échangeuse d'ions disposée entre la demi-cellule anodique (2) et la demi-cellule cathodique (3),
    l'anode (21) et/ou la cathode (31) étant des électrodes à diffusion de gaz et un interstice (32) étant disposé entre l'électrode (31) à diffusion de gaz et la membrane (4) échangeuse d'ions,
    les demi-cellules (2, 3) dotées d'une électrode (31) à diffusion de gaz présentant une amenée d'électrolyte (33) et une sortie d'électrolyte (34) ainsi qu'une entrée de gaz (35) et qu'une sortie de gaz (36),
    caractérisé en ce que
    l'électrolyte s'écoule du haut vers le bas dans l'interstice (32) au moyen d'une pompe, l'interstice (32) étant entièrement rempli d'électrolyte,
    en ce qu'un espace de gaz (37) est disposé en aval de l'électrode (31) à diffusion de gaz et
    en ce que l'espace de gaz (37) présente une entrée de gaz (35) et une sortie de gaz (36) pour le gaz de réaction.
EP04740955.2A 2003-07-24 2004-07-13 Cellule electrochimique Expired - Lifetime EP1651799B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE10333853A DE10333853A1 (de) 2003-07-24 2003-07-24 Elektrochemische Zelle
PCT/EP2004/007713 WO2005012595A1 (fr) 2003-07-24 2004-07-13 Cellule electrochimique

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EP1651799A1 EP1651799A1 (fr) 2006-05-03
EP1651799B1 true EP1651799B1 (fr) 2015-05-27

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US (2) US20050029116A1 (fr)
EP (1) EP1651799B1 (fr)
JP (1) JP4680901B2 (fr)
CN (1) CN100549239C (fr)
DE (1) DE10333853A1 (fr)
HK (1) HK1097885A1 (fr)
TW (1) TWI351447B (fr)
WO (1) WO2005012595A1 (fr)

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ITMI20060726A1 (it) * 2006-04-12 2007-10-13 De Nora Elettrodi S P A Elettrodo a diffusione gassosa per celle a percolazione di elettrolita
JP4198726B2 (ja) * 2006-09-06 2008-12-17 クロリンエンジニアズ株式会社 イオン交換膜電解槽
DE102008011473A1 (de) * 2008-02-27 2009-09-03 Bayer Materialscience Ag Verfahren zur Herstellung von Polycarbonat
DE102009004031A1 (de) * 2009-01-08 2010-07-15 Bayer Technology Services Gmbh Strukturierte Gasdiffusionselektrode für Elektrolysezellen
US8266736B2 (en) * 2009-07-16 2012-09-18 Watkins Manufacturing Corporation Drop-in chlorinator for portable spas
US8273254B2 (en) 2010-04-19 2012-09-25 Watkins Manufacturing Corporation Spa water sanitizing system
US9478803B2 (en) * 2011-06-27 2016-10-25 Primus Power Corporation Electrolyte flow configuration for a metal-halogen flow battery
GB2539478B (en) * 2015-06-17 2017-11-22 Siemens Ag Electrochemical cell and process
AU2017233774A1 (en) * 2016-03-17 2018-09-13 Hpnow Aps Electrochemical cell for gas-phase reactant in liquid environment
WO2017174563A1 (fr) 2016-04-07 2017-10-12 Covestro Deutschland Ag Électrode bifonctionnelle et dispositif d'électrolyse pour l'électrolyse de chlore-alcali
US11407661B2 (en) 2017-07-17 2022-08-09 Watkins Manufacturing Corporation Chlorine generator system
EP3805429A1 (fr) * 2019-10-08 2021-04-14 Covestro Deutschland AG Procédé et dispositif d'électrolyse destinés à la fabrication de chlore, de monoxyde de carbone et, le cas échéant, d'hydrogène

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WO2004040040A1 (fr) * 2002-10-23 2004-05-13 Uhdenora Technologies S.R.L. Cellule d'electrolyse comprenant une rigole interieure

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DE4306889C1 (de) * 1993-03-05 1994-08-18 Heraeus Elektrochemie Elektrodenanordnung für gasbildende elektrolytische Prozesse in Membran-Zellen und deren Verwendung
DE19646950A1 (de) * 1996-11-13 1998-05-14 Bayer Ag Elektrochemische Gasdiffusionshalbzelle
JP3553775B2 (ja) * 1997-10-16 2004-08-11 ペルメレック電極株式会社 ガス拡散電極を使用する電解槽
DE69929442T2 (de) * 1998-08-25 2006-08-24 Toagosei Co., Ltd. Elektrolytische sodazelle mit gasdiffusionselektrode
JP3086853B2 (ja) * 1999-02-25 2000-09-11 長一 古屋 電解槽
IT1317753B1 (it) * 2000-02-02 2003-07-15 Nora S P A Ora De Nora Impiant Cella di elettrolisi con elettrodo a diffusione di gas.
JP2001300537A (ja) * 2000-04-25 2001-10-30 Matsushita Electric Works Ltd 水浄化装置
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Publication number Priority date Publication date Assignee Title
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JP4680901B2 (ja) 2011-05-11
CN100549239C (zh) 2009-10-14
TWI351447B (en) 2011-11-01
US20050029116A1 (en) 2005-02-10
JP2006528730A (ja) 2006-12-21
CN1829825A (zh) 2006-09-06
WO2005012595A1 (fr) 2005-02-10
HK1097885A1 (en) 2007-07-06
TW200519233A (en) 2005-06-16
US20110073491A1 (en) 2011-03-31
EP1651799A1 (fr) 2006-05-03
DE10333853A1 (de) 2005-02-24

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