EP2436804A1 - Mit einer gasdiffusionselektrode und einer ionenaustauschmembran ausgestattete elektrolysezelle - Google Patents

Mit einer gasdiffusionselektrode und einer ionenaustauschmembran ausgestattete elektrolysezelle Download PDF

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Publication number
EP2436804A1
EP2436804A1 EP10780245A EP10780245A EP2436804A1 EP 2436804 A1 EP2436804 A1 EP 2436804A1 EP 10780245 A EP10780245 A EP 10780245A EP 10780245 A EP10780245 A EP 10780245A EP 2436804 A1 EP2436804 A1 EP 2436804A1
Authority
EP
European Patent Office
Prior art keywords
gas diffusion
diffusion electrode
exchange membrane
ion exchange
back plate
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Withdrawn
Application number
EP10780245A
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English (en)
French (fr)
Other versions
EP2436804A4 (de
Inventor
Kiyohito Asaumi
Yukinori Iguchi
Mitsuharu Hamamori
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.)
Toagosei Co Ltd
Kaneka Corp
ThyssenKrupp Uhde Chlorine Engineers Japan Ltd
Original Assignee
Chlorine Engineers Corp Ltd
Toagosei Co Ltd
Kaneka Corp
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 Chlorine Engineers Corp Ltd, Toagosei Co Ltd, Kaneka Corp filed Critical Chlorine Engineers Corp Ltd
Publication of EP2436804A1 publication Critical patent/EP2436804A1/de
Publication of EP2436804A4 publication Critical patent/EP2436804A4/de
Withdrawn legal-status Critical Current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
    • 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
    • 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
    • C25B9/60—Constructional parts of cells
    • C25B9/65—Means for supplying current; Electrode connections; Electric inter-cell connections

Definitions

  • the present invention relates to a gas diffusion electrode equipped ion exchange membrane electrolyzer for use in electrolysis of an alkali metal chloride aqueous solution such as brine and, more particularly, to a gas diffusion electrode equipped ion exchange membrane electrolyzer suitably applied to a two-chamber type gas diffusion electrode equipped ion exchange membrane electrolyzer.
  • a gas diffusion electrode equipped ion exchange membrane electrolyzer provided with a gas diffusion electrode is utilized as a means for reducing electrolysis voltage by causing a reaction with a gas introduced from outside at the gas diffusion electrode.
  • a gas diffusion electrode equipped ion exchange membrane electrolyzer for alkali metal chloride aqueous solution wherein the gas diffusion electrode is used as a cathode, an alkali chloride aqueous solution is supplied to an anode chamber so as to generate a chlorine gas at an anode.
  • an oxygen-containing gas is supplied to a cathode chamber, whereby at the gas diffusion electrode, the oxygen is reduced, and further, an alkali metal hydroxide aqueous solution is generated.
  • An electrolyte cannot be made to flow over the entire surface of the gas diffusion electrode unless a state where the gas diffusion electrode is brought into firm and uniform contact to the ion exchange membrane is maintained. If not, a current cannot be made to flow uniformly through the electrolytic surface of the gas diffusion electrode.
  • an ion exchange membrane electrolyzer in which a gas-permeable elastic member is disposed between a cathode chamber at the back of the gas diffusion electrode and a back plate so as to bring the gas diffusion electrode into firm contact with the ion exchange membrane and to ensure electrical conduction between the back plate of the cathode chamber and gas diffusion electrode.
  • the cathode chamber is made of nickel, a nickel alloy, or the like.
  • a passivation film is formed on the surface of the nickel or nickel alloy due to oxidation.
  • progression of metal corrosion can be restrained by the passivation film formed on the nickel or nickel alloy, a large conduction resistance is generated by the passivation film in a conducting circuit through which a current is made to flow by the contact of the elastic member with the back plate of the cathode chamber and the gas diffusion electrode.
  • Patent Document 1 To prevent a reduction in the conductivity due to the passivation film, there has been proposed a configuration in which silver plating is applied to the back plate of the cathode chamber and elastic member so as to prevent an increase in the conduction resistance (refer to e.g., Patent Document 1).
  • Patent Document 1 JP-A-2006-322018
  • An object of the present invention is to provide a gas diffusion electrode equipped ion exchange membrane electrolyzer capable of preventing an increase in the voltage of the electrolyzer due to an increase in the conduction resistance in the conducting circuit from the gas diffusion electrode to the back plate of the cathode chamber so as to perform a lower voltage operation which is one of the features of the gas diffusion electrode equipped ion exchange membrane electrolyzer for a long period of time.
  • a gas diffusion electrode equipped ion exchange membrane electrolyzer having an anode, an ion exchange membrane, and a cathode chamber in which a gas diffusion electrode is disposed, characterized in that in a cathode gas chamber formed between a back plate of the cathode chamber and one side of the gas diffusion electrode opposite to the electrolytic surface, a gas-permeable elastic member is disposed between the gas diffusion electrode and the back plate, and the elastic member forms a conductive connection between the gas diffusion electrode and the back plate by making contact with corrosion-resistant conductive layers formed on the surfaces of a plurality of conductive members which are joined to the back plate.
  • the conductive member has a silver or platinum group metal-containing corrosion-resistant conductive layer on a foil or plate made of nickel or a nickel alloy.
  • the conductive member is obtained by integrating the silver or platinum group metal-containing corrosion-resistant conductive layer by means of plating, cladding or baking coating. A part of or the entire conductive member is joined to the back plate.
  • the elastic member forms a corrosion-resistant conductive layer on a conductive contacting surface or the entire surface thereof.
  • the gas diffusion electrode equipped ion exchange membrane electrolyzer according to the present invention has a configuration in which the plurality of conductive members on the surface of each of which the corrosion-resistant conductive layer is formed are disposed on the surfaces contacting the elastic member and back plate of the cathode chamber for electrical conduction to the gas diffusion electrode.
  • a problem caused by directly plating a conductive layer to the back plate is solved as follows. That is, a plurality of conductive members made of a planar metal foil or metal plate formed by plating a corrosion-resistant conductive layer made of silver or platinum-group metal to the surface thereof are joined to the back plate so as to make the characteristics of the contacting portion to an elastic member uniform, thereby allowing prevention of a phenomenon such as separation of the corrosion-resistant conductive layer contacting the elastic member.
  • FIG. 1 is a cross-sectional view for explaining an embodiment of a gas diffusion electrode equipped ion exchange membrane electrolyzer according to the present invention. The following description is made taking a gas diffusion electrode equipped ion exchange membrane electrolyzer for use in electrolysis of brine, in which a single anode chamber and a single cathode chamber are stacked through an ion exchange membrane.
  • FIG. 1 is a cross-sectional view obtained by cutting the gas diffusion electrode equipped ion exchange membrane electrolyzer along a plane orthogonal to an electrode surface.
  • a gas diffusion electrode equipped ion exchange membrane electrolyzer 1 has a configuration called a two-chamber type gas diffusion electrode equipped ion exchange membrane electrolyzer, in which an anode chamber 20 and a cathode chamber 30 provided therein are separated by an ion exchange membrane 10.
  • the anode chamber 20 has an anode 211 and is filled with brine as an anolyte 213.
  • An anolyte inlet 215 is formed at the lower portion of the anode chamber 20.
  • An outlet 217 for anolyte whose concentration has been decreased by electrolysis and gas is formed at the upper portion of the anode chamber, and an anode chamber frame 219 is stacked to the ion exchange membrane 10 through an anode chamber side gasket 221.
  • the cathode chamber 30 is provided on the opposite side to the anode chamber 20 with respect to the ion exchange membrane 10, and a gas diffusion electrode 313 is provided in the cathode chamber.
  • a liquid retaining member 311 is disposed between a cathode chamber inner space 301 including the gas diffusion electrode 313 and ion exchange membrane 10.
  • an elastic member 330 which is made of a wire rod and which has inside thereof a space through which a gas can be passed is disposed.
  • the elastic member 330 brings the gas diffusion electrode 313 and liquid retaining member 311 into firm contact with the ion exchange membrane 10 side to form a cathode gas chamber 317 within the cathode chamber and makes contact with corrosion-resistant conductive layers 341 formed on the surfaces of a plurality of conductive members 340 which are joined to the back plate 327 of the cathode chamber 30 to form a conducting circuit between the gas diffusion electrode 313 and back plate 327.
  • the generated alkali metal hydroxide aqueous solution is transferred to the liquid retaining member 311 according to the concentration gradient and absorbed/retained by the liquid retaining member 311, as well as flows down along the inside of the liquid retaining member 311 and gas chamber side of the gas diffusion electrode 313 to be discharged from a cathode gas chamber outlet 321.
  • the cathode chamber is made of nickel, a nickel alloy, or the like.
  • the elastic member is made of a metal material having a high corrosion resistance and a high conductivity, such as nickel or a high nickel alloy.
  • a metal having a satisfactory corrosion resistance such as nickel or a nickel alloy, used as a material of the cathode gas chamber 317 is oxidized at its surface in the presence of a high concentration oxygen to form a passivation film, impeding electrical conduction, which leads to an increase in the voltage of the electrolyzer.
  • a plurality of planar conductive members 340 each having a corrosion-resistant conductive layer 341 on the surface thereof are disposed on the back plate 327 of the cathode chamber 30.
  • Each planar conductive member 340 has the corrosion-resistant conductive layer 341 whose surface characteristics are made uniform by plating, cladding, or baking coating, so that even if the area of the back plate 327 is increased, a surface having uniform characteristics can be obtained in any position.
  • planar conductive member it is preferable to use the same material as that of the back plate of the cathode chamber, i.e., a nickel material, the thickness thereof preferably being 0.1 mm to 1.0 mm.
  • the corrosion-resistant conductive layer may be formed of a metal such as silver or platinum group metal and it is particularly preferable to use silver having a satisfactory conductivity.
  • the corrosion-resistant conductive layer can be formed by plating, cladding, baking, or the like.
  • the thickness of the corrosion-resistant conductive layer is preferably set to 0.5 ⁇ m or more. When the thickness falls below 0.5 ⁇ m, sufficient characteristics cannot be obtained.
  • the planar conductive member is formed in a size of 60 mm ⁇ 56 mm to 1220 mm ⁇ 500 mm.
  • the size is smaller than 60 mm ⁇ 56 mm, the number of the planar conductive members to be installed is increased to increase the number of spot welding points, which may result in a degradation of the uniformity.
  • the size is larger than 1220 mm ⁇ 500 mm, nonuniformity is likely to occur unfavorably when the corrosion-resistant conductive layer is formed by plating or the like.
  • FIG. 2 is a view for explaining the embodiment of the gas diffusion electrode equipped ion exchange membrane electrolyzer according to the present invention and more specifically, an exploded perspective view for explaining the elastic member and conductive member.
  • the plurality of conductive members 340 are joined to the back plate 327 of a cathode chamber frame 323.
  • 12 conductive members 340 are disposed.
  • the elastic member 330 is disposed such that one surface thereof contacts the conductive members 340 and the other surface thereof contacts one surface of the gas diffusion electrode opposite to the electrolytic surface.
  • FIG. 1 is a view for explaining the embodiment of the gas diffusion electrode equipped ion exchange membrane electrolyzer according to the present invention and more specifically, an exploded perspective view for explaining the elastic member and conductive member.
  • the plurality of conductive members 340 are joined to the back plate 327 of a cathode chamber frame 323.
  • 12 conductive members 340 are disposed.
  • the elastic member 330 is disposed such that one surface thereof contacts the conductive members 340 and the other surface thereof contacts
  • the elastic member 330 has eight unit elastic members 333a, 333b, 333c, 333d, 333e, 333f, 333g, and 333h mounted to an elastic member frame 331, each of which is constituted by a hollow spring coil forming a gas passage and is disposed so as to uniformly press the gas diffusion electrode and to allow uniform electrical conduction between the gas diffusion electrode and back plate.
  • the use of the plurality of unit elastic members can allow the pressure and current distribution uniformly applied to the gas diffusion electrode even when the electrolysis area of the gas diffusion electrode is increased.
  • the number of the unit elastic members 333a to 333h forming the elastic member 330 and the number of the conductive members may appropriately be set in accordance with the size of the electrolysis area or magnitude of the application current density.
  • FIG. 3 is a view for explaining the embodiment of the gas diffusion electrode equipped ion exchange membrane electrolyzer according to the present invention, which illustrates the conductive member.
  • conductive members 340 each having a comparatively large area are mounted to the back plate by a method such as spot welding performed at joining portions 343 and the corrosion-resistant conductive layers 341 formed on the conductive members 340 are disposed on the gas diffusion electrode side.
  • a large number of conductive members 340 each having a smaller area than the conductive members of FIG. 3A are mounted to the back plate 327 and joined thereto at the joining portions 343, and corrosion-resistant conductive layers 341 are formed respectively on the surface of the mounted conductive members.
  • the mounting of a large number of the small-area conductive members 340 allows stable electrical conduction between the back plate and gas diffusion electrode for a long period of time.
  • the present invention will be described based on Examples and Comparative Examples.
  • An ion exchange membrane (anode ion exchange membrane F-8020 made by Asahi Glass Co., Ltd) was disposed in an electrolyzer having an effective electrolysis area of 56 mm (height) ⁇ 60 mm (width) so as to contact an anode for brine electrolysis (JP202R made by Permelec Electrode Ltd.).
  • a carbon fiber fabric (made by Zoltek) having a thickness of 0.4 mm that covers the electrolytic surface was stacked as a liquid retaining member, and further a liquid-permeable gas diffusion electrode (Permelec Electrode Ltd.) was stacked on the liquid retaining member.
  • a nickel wire coil obtained by winding a nickel wire having a wire diameter of 0.17 mm in a coil shape having a winding diameter of 6 mm was disposed on one side of the gas diffusion electrode opposite to the electrolytic surface.
  • a conductive member made of a nickel foil (NW2201) of 56 mm (H)x 60 mm (W) ⁇ 0.2 mm (T) having one surface that has been subjected to silver plating was joined to the back plate of the cathode chamber of the cathode chamber frame by spot welding at six points.
  • a voltage measurement terminal was attached to the gas diffusion electrode, and the electrolyzer was operated for 17 days with the current density kept at 3 kA/m 2 , electrolysis temperature kept at 87°C to 89°C, and aqueous sodium hydroxide concentration kept at 30 mass% to 33 mass%.
  • a potential difference between the gas diffusion electrode and back plate, i.e., voltage drop was measured. The measurement result is shown in FIG. 4 .
  • a voltage was not increased but kept at an initial voltage of 0.001 V, that is, operation of the electrolyzer was stable for 17 days.
  • An ion exchange membrane (anode ion exchange membrane "Aciplex" F-4403 made by Asahi Kasei Chemicals Corporation) was disposed in an electrolyzer having an effective electrolysis area of 620 mm (width) ⁇ 1220 mm (height) so as to contact an anode for brine electrolysis (JP202R made by Permelec Electrode Ltd.).
  • a carbon fiber fabric (made by Zoltek) having a thickness of 0.4 mm that covers the electrolytic surface was stacked as a liquid retaining member, and further a liquid-permeable gas diffusion electrode (Permelec Electrode Ltd.) was stacked on the liquid retaining member.
  • electrolyzer was used to perform electrolysis with the current density kept at 3 kA/m 2 , electrolysis temperature kept at 75°C to 85°C, and aqueous sodium hydroxide concentration kept at 30 mass% to 34 mass%. As illustrated in FIG. 5 showing a trend in the voltage of the electrolyzer, an increase in the voltage was not observed. when the electrolyzer was disassembled after the total operation period of 500 days, no abnormality was observed in the silver plated conductive member.
  • Example 1 An electrolyzer produced in the same manner as Example 1 except that the silver plating was not applied to the conductive member was used to perform electrolysis under the same conditions as those in Example 1, and a potential difference between the gas diffusion electrode and back plate of the cathode chamber was measured in the same manner as Example 1. As illustrated in FIG. 4 showing the measurement result, the potential difference was increased with time. Further, when the electrolyzer was disassembled after stop of the operation, the nickel foil used as the conducting member was turned black due to formation of a passivation film.
  • Electrolysis was performed in the same manner as Example 2 except that an electrolyzer has a cathode chamber in which the conductive member was not provided and silver plating of a 10 ⁇ m center thickness was applied to the back plate, and a trend in the voltage of the electrolyzer was measured. A 200 mV voltage increase was observed after 300 days operation. Further, when the electrolyzer was disassembled after stop of the operation, the silver plating at substantially all the conducting portions of the silver plating layer of the back plate contacting the elastic member were separated to expose the nickel material as the underlayer, and further, the nickel material as the underlayer was turned black due to formation of a passivation film.
  • the gas diffusion electrode equipped ion exchange membrane electrolyzer according to the present invention has a configuration in which the plurality of conductive members on the surface of each of which the corrosion-resistant conductive layer is formed are disposed on the surfaces contacting the elastic member and back plate of the cathode chamber for electrical conduction to the gas diffusion electrode.
  • a gas diffusion electrode equipped ion exchange membrane electrolyzer in which characteristics of the contact portion with the elastic member for electrical conduction to the gas diffusion electrode are stable, no separation of the corrosion-resistant conductive layer from the surface of the conductive member occurs, voltage drop between the gas diffusion electrode and back plate is small, and performance can be made stable for a long period of time.

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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)
EP10780245.6A 2009-05-26 2010-05-24 Mit einer gasdiffusionselektrode und einer ionenaustauschmembran ausgestattete elektrolysezelle Withdrawn EP2436804A4 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
JP2009126622 2009-05-26
PCT/JP2010/003470 WO2010137284A1 (ja) 2009-05-26 2010-05-24 ガス拡散電極装着イオン交換膜電解槽

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EP2436804A1 true EP2436804A1 (de) 2012-04-04
EP2436804A4 EP2436804A4 (de) 2015-05-27

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US (1) US20120125782A1 (de)
EP (1) EP2436804A4 (de)
JP (1) JP5785492B2 (de)
CN (1) CN102459708A (de)
WO (1) WO2010137284A1 (de)

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2957659A1 (de) 2014-06-16 2015-12-23 Siemens Aktiengesellschaft Gasdiffusionsschicht, PEM-Elektrolysezelle mit einer solchen Gasdiffusionsschicht sowie Elektrolyseur
WO2021110457A1 (de) 2019-12-06 2021-06-10 Thyssenkrupp Uhde Chlorine Engineers Gmbh Verwendung eines textils, zero-gap-elektrolysezelle und herstellungsverfahren dafür

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102011008163A1 (de) * 2011-01-10 2012-07-12 Bayer Material Science Ag Beschichtung für metallische Zellelement-Werkstoffe einer Elektrolysezelle
JP5970250B2 (ja) 2012-06-13 2016-08-17 ティッセンクルップ・ウーデ・クロリンエンジニアズ株式会社 イオン交換膜電解槽用弾性クッション材
WO2015114917A1 (ja) * 2014-01-29 2015-08-06 株式会社島津製作所 金属電極、それを用いた電子銃、電子管並びにｘ線管
CN113957466B (zh) * 2021-11-08 2023-03-14 中国石油大学(华东) 光电催化反应用流动式电解池

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JP3437123B2 (ja) * 1999-06-18 2003-08-18 鐘淵化学工業株式会社 イオン交換膜型電解槽及び電解方法
DE10138214A1 (de) * 2001-08-03 2003-02-20 Bayer Ag Elektrolysezelle und Verfahren zur elektrochemischen Herstellung von Chlor
DE10159708A1 (de) * 2001-12-05 2003-06-18 Bayer Ag Alkalichlorid-Elektrolysezelle mit Gasdiffusionselektroden
EP1378589B1 (de) * 2002-04-05 2005-12-07 CHLORINE ENGINEERS CORP., Ltd. Ionenaustauschermembran-Elektrolyseur
JP3924545B2 (ja) * 2003-03-31 2007-06-06 三井化学株式会社 ガス拡散電極の排電方法
JP4834329B2 (ja) 2005-05-17 2011-12-14 クロリンエンジニアズ株式会社 イオン交換膜型電解槽
ITMI20060054A1 (it) * 2006-01-16 2007-07-17 Uhdenora Spa Distributore di corrente elastico per celle a percolatore

Non-Patent Citations (1)

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Title
See references of WO2010137284A1 *

Cited By (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP2957659A1 (de) 2014-06-16 2015-12-23 Siemens Aktiengesellschaft Gasdiffusionsschicht, PEM-Elektrolysezelle mit einer solchen Gasdiffusionsschicht sowie Elektrolyseur
US10294572B2 (en) 2014-06-16 2019-05-21 Siemens Aktiengesellschaft Gas diffusion layer, electrochemical cell having such a gas diffusion layer, and electrolyzer
WO2021110457A1 (de) 2019-12-06 2021-06-10 Thyssenkrupp Uhde Chlorine Engineers Gmbh Verwendung eines textils, zero-gap-elektrolysezelle und herstellungsverfahren dafür

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WO2010137284A1 (ja) 2010-12-02
JPWO2010137284A1 (ja) 2012-11-12
JP5785492B2 (ja) 2015-09-30
EP2436804A4 (de) 2015-05-27
US20120125782A1 (en) 2012-05-24
CN102459708A (zh) 2012-05-16

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