WO2002103082A1 - Cellule d'electrolyse - Google Patents

Cellule d'electrolyse Download PDF

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Publication number
WO2002103082A1
WO2002103082A1 PCT/SE2002/000869 SE0200869W WO02103082A1 WO 2002103082 A1 WO2002103082 A1 WO 2002103082A1 SE 0200869 W SE0200869 W SE 0200869W WO 02103082 A1 WO02103082 A1 WO 02103082A1
Authority
WO
WIPO (PCT)
Prior art keywords
gas diffusion
electrolytic cell
diffusion electrode
members
electrode members
Prior art date
Application number
PCT/SE2002/000869
Other languages
English (en)
Inventor
Takayuki Shimamune
Original Assignee
Akzo Nobel N.V.
Eka Chemicals Ab
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 Akzo Nobel N.V., Eka Chemicals Ab filed Critical Akzo Nobel N.V.
Priority to EP02728293A priority Critical patent/EP1397531A1/fr
Publication of WO2002103082A1 publication Critical patent/WO2002103082A1/fr

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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
    • 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
    • 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

  • Electrolytic cell The invention relates to an electrolytic cell suitable for producing alkali metal hydroxide and the use of such cell.
  • the invention also relates to a method for manufacturing such cell.
  • reaction (1) is replaced by reaction (2) as follows:
  • US 5,938,901 discloses an electrolytic cell partitioned by an ion exchange membrane into an anode chamber and a cathode chamber.
  • the electrolytic cell comprises current collectors electrically connected to horizontal electrode members having the shape of belts arranged with a space between the members in the vertical direction, which electrode members are contacted to the membrane.
  • the present invention relates to an electrolytic cell comprising an anode and a cathode compartment, a separator partitioning the compartments, gas diffusion electrode members arranged to said separator with a space between electrode members in the vertical direction.
  • the cell further comprises current collector members electrically connected to the electrode members.
  • the current collector members comprise resilient means arranged to homogenise the contact between the electrode members, the current collector and the separator.
  • the present invention can maintain the operation of an electrolytic cell at a low and stable cell voltage due to the improved contact between the current collector, the gas diffusion electrode, and the separator. Moreover, it has been found that the invention solves the technical problem of unwanted drying, and flooding of electrolyte in the cathode compartment. The present invention also solves the technical problem of supplying oxygen-containing gas to the gas diffusion electrode in an effective way.
  • the electrode members are suitably shaped as belts, preferably as substantially squares.
  • the electrode members have a length of from “ about 2 to about 40 cm, preferably from about 10 to about 30 cm in the vertical direction in a conventional electrolytic cell of ordinary size. If the vertical length is less than about 2 cm, the preparation of the electrode members can be complicated. If the vertical length is longer than about 40 cm, the lower portion of the electrode member may be exposed to an excess of electrolyte, which will reduce the rate of the electrolytic reaction taking place at the gas diffusion electrode due to blockage of oxygen-containing gas supply caused by flooding of electrolyte.
  • the electrode members have a length of from about 2 to about 40 cm, preferably from about 10 to about 30 cm, in the horizontal direction in a conventional electrolytic cell of ordinary size.
  • the space between the electrode members in the vertical direction may be appropriately selected in a range such that the reduction of electrolytic area is restrained and the release of electrolyte is smoothly carried out. It is highly advantageous that oxygen supplied to the cathode compartment is not hindered by remaining electrolyte on the electrode from diffusing into the gas diffusion electrode via the gas diffusion layer provided on the side facing away from the separator.
  • the space between the electrode members in the vertical direction may be from about 1 to about 5 mm, preferably from about 2 to about 3 mm.
  • An electrolyte is allowed to flow downwards on the surface of each electrode member by gravity until it reaches the lower portion thereof.
  • the space provided between the electrode members can to some extent prevent electrolyte from flowing down to the electrode member arranged underneath the foregoing electrode member.
  • the electrolyte can partially flow along the space extending in the horizontal direction and further down to the bottom of the electrolytic cell.
  • At least one electrolyte guide plate can be attached to an electrode member or between the electrode members in the vertical direction such that the guide plate is downwardly inclined to the opposite side of the separator.
  • the electrolyte guide plate is preferably provided in the space between the vertically arranged electrode members.
  • the electrolyte guide plate prevents electrolyte from flowing downwardly to the next-coming electrode members by guiding the electrolyte away from the electrode members underneath.
  • the electrolyte guide plates suitably have a length from about 1 to about 3 mm, preferably from about 2 to about 3 mm.
  • the electrolyte guide plates are prepared by moulding a corrosion resistant resin, such as a fluorine resin, polyethylene, polypropylene, or other suitable resins.
  • a corrosion resistant resin such as a fluorine resin, polyethylene, polypropylene, or other suitable resins.
  • the electrolyte guide plates may also be prepared by moulding a metal.
  • the electrode members themselves can also be downwardly inclined to the opposite side of the separator in the lower portion to prevent flooding of electrolyte.
  • each of the electrode members are downwardly inclined to the opposite side of the separator.
  • a space is also provided between electrode members in the horizontal direction.
  • the electrode members do not necessarily continue over the whole horizontal direction in the cell, but may be divided into plural parts in the horizontal direction.
  • electrolyte can flow down from each space formed by the horizontal division.
  • electrolyte can easily be released from the electrode members.
  • the structure of plural electrode members arranged both in the horizontal direction and the vertical direction with a space in between can be described as a patchwork.
  • the space between the electrode members in the horizontal direction is from about 1 to about 5 mm, preferably from about 2 to about 3 mm. The space between the electrode members cannot be employed for electrolysis.
  • electrolysis processes are carried out on a reaction layer of the gas diffusion electrode, electrolyte can permeate through the surface of the gas diffusion layer.
  • sodium hydroxide is being produced in the electrolytic cell, sodium ions and water from the anode compartment, which are supplied thereto as an aqueous sodium chloride solution, are transported via the separator to the reaction layer of the gas diffusion electrode.
  • Oxygen-containing gas is led into the cathode compartment and supplied to the reaction layer via the gas diffusion layer so that it can react with water. Hydroxyl ions are thus formed, which subsequently react with sodium ions to form sodium hydroxide.
  • separator any separating means, such as an ion exchange membrane, a diaphragm or other separating means.
  • Suitable membranes may be made of perfluorinated, sulphonated or teflon-based polymers, or ceramics. Also polystyrene-based membranes or diaphragm of polymers or ceramics may be used. There are several commercially available membranes suitable for use such as NafionTM 324, NafionTM 550 and NafionTM 961 by Du Pont or FlemionTM by Asahi Glass.
  • the gas diffusion electrode members are electrically connected to current collector members, which supply electric current to the electrode members.
  • the current collector members can be connected to the electrode members in various manners, e.g. by spot welding or wiring thereto.
  • the current collector members and the gas diffusion electrode members may also be contacted frictionally without any further contacting means to ascertain electrical contact.
  • the current collector comprising plural current collector members is suitably made of a porous metal, e.g. expanded mesh, perforated or louvered plates so that gas and electrolytes thereby easily can be supplied and removed from the gas diffusion electrode members.
  • the current collector members are suitably arranged to the wall opposite to the separator in the cathode compartment by resilient means, e.g. U or V- shaped springs or ribs, elastic louvers, or other elastic material.
  • the area of the current collector members contacted to the gas diffusion electrode members have the shape of a square or a rectangle adapted to the dimensions of the gas diffusion electrode members.
  • the current collector members have substantially the same dimensions as the gas diffusion electrode members so that they can be individually fitted thereto.
  • the sides, i.e. the lengths or dimensions in the vertical and horizontal direction, of the current collector members connected to the gas diffusion electrode members are suitably not larger than 40 cm, because the homogeneous contact with the membrane can in those cases be insufficient, which can lead to inhomogeneous current distribution
  • the manufacturing of the current collector members may be very complicated.
  • the sides of the current collector members are suitably from about 10 to about 40 cm, preferably from, about 10 to about 30 cm, and most preferably from about 20 to about 25 cm.
  • the space between the current collector members is suitably from about 3 to about 10 mm, preferably from about 4 to about 6 mm. In case the space is too big, the cell voltage may be too high due to inhomogeneous current distribution in the cell. If the space is too small, the independent adjustments of the electrode members to the current collectors may be difficult.
  • the electrolytic cell is a conventional cell comprising an existing hydrogen-evolving cathode, hereinafter called existing cathode, which has been retrofitted with gas diffusion electrode members.
  • the electrolytic cell can thus be a retrofitted cell further comprising a hydrogen evolving cathode electrically arranged between the gas diffusion electrode and the current collector members.
  • the gas diffusion electrode members can be arranged on the side of the existing cathode facing the separator.
  • the existing cathode can then be used as current collector means to transfer current to the gas diffusion electrode.
  • Slits in the horizontal direction are suitably made in the existing cathode to form plural cathode members, in such a way that the lower portion of the gas diffusion electrode members can be passed through the slits so that electrolyte can be eliminated from the gas diffusion electrode members.
  • a space can thus be formed between the existing cathode members in the vertical direction.
  • the distance between each slit suitably is from about 10 to about 40 cm, preferably from about 20 to 30 cm.
  • the space between the vertical existing cathode members suitably is from about 3 to about 10 mm.
  • the gas diffusion electrode members are welded to the existing cathode members.
  • the current collector members are suitably arranged, suitably by means of welding so that a homogeneous contact can be secured.
  • the shape of the existing cathode members suitably have about the same dimensions as the gas diffusion electrode members electrically arranged thereto.
  • the gas diffusion electrode comprising several electrode members, is a gas diffusion cathode.
  • the gas diffusion electrode of the present invention is suitably obtained by sintering a silver powder on a surface of a gas-liquid permeable metal substrate such as a perforated plate, an expanded mesh, a metal foam, a sintered metal, a metal fibre structural material, or the like.
  • the metal substrate can comprise silver alone, silver-plated copper or nickel or a mixture thereof.
  • a thin layer comprising a carbon powder and a silver fibre having perforations in the thickness direction can then be formed on the surface of the metal substrate.
  • the thin layer may be further subjected to fluorination treatment to fluorinate the carbon in the thin layer.
  • a thin layer may be prepared by baking a paste obtained by kneading a silver powder and a fluorinated carbon compound such as a PTFE (polytetrafluoroethylene) resin at a temperature of from about 150 °C to about 350 °C.
  • a fluorinated carbon compound such as a PTFE (polytetrafluoroethylene) resin
  • the sintering method is optional and, for example, a silver powder having a particle size of from about 1 to about 10 ⁇ m is kneaded with a material such as dextrin, which functions as a binder and is evaporated off by sintering or burning.
  • the coated substrate can be sintered in air or in a weakly reducing atmosphere such as a hydrogen gas atmosphere at a temperature of from about 300 °C to about 600 °C.
  • the gas diffusion electrode thus prepared has sufficient catalytic activity as it is but an active catalyst such as platinum may be carried on the surface thereof.
  • a butyl alcohol solution of chloroplatinic acid may be coated on the opposite side of the coated side of the substrate, followed by heat-treating of the coated metal substrate in a hydrogen gas atmosphere at a temperature of from about 150 °C to about 250 °C.
  • the surface of the gas diffusion layer is preferably hydrophilic, and sometimes removal of the electrolyte cannot be smoothly carried out as a result.
  • PTFE resin solution be coated on the surface of the gas diffusion layer and baked at a temperature of from about 150 °C to about 250 °C to impart a hydrophobic property to the gas diffusion layer.
  • the gas diffusion electrode is prepared from a silver expanded mesh, which is suitably degreased and pickled in a mineral acid such as nitric acid.
  • a silver paste obtained from a silver powder of 0.5-2 ⁇ m particles mixed with e.g. glucose and water, can be applied to the expanded mesh.
  • the silver paste-mesh is then suitably sintered at a temperature of about 450 °C in air.
  • a di-nitro di- amino platinum solution can then be applied on one side of the sintered silver mesh and baked at a temperature of 350 °C to form a platinum coating on the silver mesh.
  • a tetra butyl zirconate alcohol solution can be applied followed by baking at 450 °C in air atmosphere to form a zirconium dioxide coating upon the platinum coating.
  • a 0.2 mm graphite cloth can then be applied on the zirconium dioxide layer to provide a path layer.
  • the path layer keeps electrolyte in between the reaction layer of the gas diffusion electrode and the separator so as to drain the electrolyte properly which avoids flooding of the gas diffusion layer.
  • the path layer can prevent the hydrophilic reaction layer of the gas diffusion electrode from becoming hydrophobic.
  • another layer of zirconium dioxide can be applied.
  • a PTFE solution can be applied and baked at 250 °C to provide a gas diffusion layer.
  • a path layer can also be separately arranged to the gas diffusion electrode, i.e. without being integrated in the gas diffusion electrode structure. It has been found that substantially no flooding occurs even though a relatively thin path layer is applied to the gas diffusion electrode. If the path layer is separately arranged to the gas diffusion electrode members, the path layer must be downwardly inclined opposite to the separator in the embodiments where the electrode members are so inclined. The path layer can be adhered on the reaction layer or adjacent to the reaction layer on the side facing towards the separator. The path layer may also be pressed between the gas diffusion electrode and the separator so no displacement thereof can occur. Preferably, the path layer is arranged to the separator with no or substantially no space in between.
  • the typical material for the path layer is carbon, carbon cloth, carbon paper or the like, or mixtures thereof.
  • Ceramic materials are especially suitable to provide a barrier between the path layer and the reaction layer in order to prevent chemical contact between carbon in the path layer and active catalytic particles present in the reaction layer which otherwise may be damaged due to chemical reactions with carbon, leading to formation of carbonates, which may render the hydrophilic reaction layer hydrophobic.
  • Other gas diffusion electrode which may be used include such as mentioned in the European patent applications no.00850191.8 and no.00850219.7, and in US 5,938,901.
  • the current density when the electrolytic cell is in operation is suitably from about 2 to about 6, preferably from about 3 to about 4 kA/m 2 .
  • the invention also relates to a method for manufacturing an improved electrolytic cell as described herein. The method involves arranging a separator to partition an electrolytic cell into an anode and a cathode compartment. Gas diffusion electrode members are arranged to the separator with a space between electrode members in the vertical direction, and current collector members comprising resilient means are electrically connected to the electrode members.
  • the invention further relates to the use of an electrolytic cell as described herein.
  • the electrolytic cell of the invention is preferably used for production of an alkali metal hydroxide such as KOH and/or NaOH, but may also be used for production of e.g. Na 2 S0 4 , HCI.
  • Fig.1 shows a front view of a cell arrangement, in which gas diffusion electrode members have the shape of belts.
  • Fig.2 shows a front view of a cell arrangement, in which gas diffusion electrode members have a patchwork structure.
  • Fig.3-6 show various resilient means arranged to a current collector.
  • fig.1 shows a gas diffusion electrode (2) attached to an ion exchange membrane (1).
  • the gas diffusion electrode comprises belt-shaped members (2) on which a plural number of current collector members (3) are arranged.
  • resilient means (4) are arranged to secure a homogeneous current distribution over the whole electrode area.
  • Fig.2 shows a gas diffusion electrode (2) attached to an ion exchange membrane (1).
  • the gas diffusion electrode comprises a plural number of electrode members (2) in arranged in the form of a patchwork attached to an ion exchange membrane (1) in the same way as in fig.1.
  • Fig.3-6 show various resilient means (4) which can be arranged to the current collector members.
  • Such resilient means can be e.g. elastic louvers (fig.3 and 4), substantially U-shaped ribs (fig.5), and substantially V-shaped ribs (fig.6).
  • Example 1 A two compartment electrolytic cell, partitioned by a nafionTM 961 cation exchange membrane available from DuPont was used for the production of sodium hydroxide.
  • the cell had a width of 40 cm, and a height of 120 cm.
  • the anode compartment was made of titanium, in which a DSATM (dimension stable anode) with expanded mesh substrate was welded to a flange and ribs in the anode compartment.
  • a DSATM dimension stable anode
  • the cathode compartment made of nickel, four rows of horizontally arranged ribs with v- shaped cross-section, imparting elastic properties to the current collectors, were welded to the bottom of the compartment. The elastic ribs were bent so they formed angles of about 45°.
  • the upper portion of the ribs were arranged at the same height at a flange.
  • the ribs were cut every 20 mm to be independently movable.
  • a gas diffusion electrode comprised four layers joined to each other in the following order: path layer of Zr0 2 -graphite, a barrier layer of Zr0 2 , a reaction layer of platinum coated silver, and a hydrophobic PTFE-silver layer being a gas diffusion layer.
  • the gas diffusion electrode was cut to the dimensions 195 (width) x 210 (height) mm to form separate electrode members. 15 mm from the lower edge, the electrode members were downwardly inclined to the direction opposite to the cation exchange membrane. The electrode members were arranged to the current collector by spot welding.
  • the electrolytic cell was fabricated by providing gas inlets and outlets, distributors, and continuous draining means for the electrolyte.
  • the electrolysis was performed by supplying 180 g litre of NaCI to the anode compartment and water-containing oxygen gas to the cathode compartment.
  • the operating temperature was 90 °C and the current density 4 kA/m 2 .
  • the electrolysis could be performed without flooding at a stable cell voltage of
  • Example 2 The electrolytic cell of example 1 was prepared in the same way, but with non- elastic ribs. When the cell was in operation, the cell voltage was unstable at a level about 2.4V. When the electrolysis process had been interrupted, the cell was opened for control. At the gas diffusion layer, electrolyte was observed due to insufficient and inhomogeneous contact between the membrane and the gas diffusion electrode. The area between the electrode members and the cation exchange membrane contained no electrolyte, and a portion of the electrode surface was dry. As a consequence, the electrolysis process suffered from a high local current density at some points because of inhomogeneous contact, and a high cell voltage.
  • Example 3 The electrolytic cell of example 1 was prepared except that only one current collector was attached to one single electrode member. Electrolysis was performed under the same conditions as in example 1 except that the current density was 2 kA/m 2 . The cell voltage obtained was 2.6 V. Flooding at the bottom of the cell occurred and a partial blinding area due to insufficient contact between the electrode and the ion exchange membrane was observed after having disassembled the cell. The flooding and the inhomogeneous contact also caused an elevated cell voltage.

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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)

Abstract

Cette invention concerne une cellule d'électrolyse ainsi qu'un procédé de fabrication de ce type de cellules. Cette cellule comprend un compartiment anodique et un compartiment cathodique, un séparateur, qui fractionne ces compartiments, des éléments électrodes de diffusion de gaz disposés sur le séparateur, un espace séparant les éléments électrodes adjacents dans la direction verticale et des éléments collecteurs de courant connectés électriquement aux éléments électrodes. Les éléments collecteurs de courant comprennent des éléments souples disposés de manière qu'ils homogénéisent le contact entre les éléments électrodes, le collecteur de courant et le séparateur. Cette invention concerne également l'utilisation de la cellule électrolytique pour la production, notamment, d'hydroxyde alcalin.
PCT/SE2002/000869 2001-06-15 2002-05-03 Cellule d'electrolyse WO2002103082A1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP02728293A EP1397531A1 (fr) 2001-06-15 2002-05-03 Cellule d'electrolyse

Applications Claiming Priority (4)

Application Number Priority Date Filing Date Title
US29809401P 2001-06-15 2001-06-15
EP01850109 2001-06-15
EP01850109.8 2001-06-15
US60/298,094 2001-06-15

Publications (1)

Publication Number Publication Date
WO2002103082A1 true WO2002103082A1 (fr) 2002-12-27

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Family Applications (1)

Application Number Title Priority Date Filing Date
PCT/SE2002/000869 WO2002103082A1 (fr) 2001-06-15 2002-05-03 Cellule d'electrolyse

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EP (1) EP1397531A1 (fr)
WO (1) WO2002103082A1 (fr)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104254644A (zh) * 2012-04-27 2014-12-31 氯工程公司 离子交换膜电解槽

Families Citing this family (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
ITMI20060054A1 (it) * 2006-01-16 2007-07-17 Uhdenora Spa Distributore di corrente elastico per celle a percolatore

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4502935A (en) * 1982-06-25 1985-03-05 Metallgesellschaft Aktiengesellschaft Electrolytic cell having a membrane and vertical electrodes
US4693797A (en) * 1979-08-03 1987-09-15 Oronzio Denora Impianti Elettrochimici S.P.A. Method of generating halogen and electrolysis cell
EP0410159A1 (fr) * 1989-07-24 1991-01-30 Asea Brown Boveri Ag Collecteur de courant pour pile à combustible fonctionnant à haute température
EP0522382A1 (fr) * 1991-06-27 1993-01-13 De Nora Permelec S.P.A. Appareil et procédé pour décomposer électrochimiquement des solutions salines en leur base et acide correspondants
US5938901A (en) * 1996-07-11 1999-08-17 Permelec Electrode Ltd. Liquid permeation-type gas-diffusion electrode

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4693797A (en) * 1979-08-03 1987-09-15 Oronzio Denora Impianti Elettrochimici S.P.A. Method of generating halogen and electrolysis cell
US4502935A (en) * 1982-06-25 1985-03-05 Metallgesellschaft Aktiengesellschaft Electrolytic cell having a membrane and vertical electrodes
EP0410159A1 (fr) * 1989-07-24 1991-01-30 Asea Brown Boveri Ag Collecteur de courant pour pile à combustible fonctionnant à haute température
EP0522382A1 (fr) * 1991-06-27 1993-01-13 De Nora Permelec S.P.A. Appareil et procédé pour décomposer électrochimiquement des solutions salines en leur base et acide correspondants
US5776328A (en) * 1991-06-27 1998-07-07 De Nora Permelec S.P.A. Apparatus and process for electrochemically decomposing salt solutions to form the relevant base and acid
US5938901A (en) * 1996-07-11 1999-08-17 Permelec Electrode Ltd. Liquid permeation-type gas-diffusion electrode

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104254644A (zh) * 2012-04-27 2014-12-31 氯工程公司 离子交换膜电解槽
EP2843084A4 (fr) * 2012-04-27 2016-04-13 Chlorine Eng Corp Ltd Cellule destinée à une électrolyse à membrane échangeuse d'ions
CN104254644B (zh) * 2012-04-27 2017-03-01 氯工程公司 离子交换膜电解槽
US9828684B2 (en) 2012-04-27 2017-11-28 Thyssenkrupp Uhde Chlorine Engineers (Japan) Ltd. Cell for ion exchange membrane electrolysis

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