EP0282614A1 - Cadre de construction pour une cellule électrochimique - Google Patents

Cadre de construction pour une cellule électrochimique Download PDF

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Publication number
EP0282614A1
EP0282614A1 EP87103843A EP87103843A EP0282614A1 EP 0282614 A1 EP0282614 A1 EP 0282614A1 EP 87103843 A EP87103843 A EP 87103843A EP 87103843 A EP87103843 A EP 87103843A EP 0282614 A1 EP0282614 A1 EP 0282614A1
Authority
EP
European Patent Office
Prior art keywords
planar member
structural frame
liner
cell
anolyte
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Withdrawn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
EP87103843A
Other languages
German (de)
English (en)
Inventor
Richard N. Beaver
Hiep D. Dang
Gregory J.E. Morris
John R. Pimlott
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.)
Dow Chemical Co
Original Assignee
Dow Chemical Co
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
Priority to US06/809,372 priority Critical patent/US4666580A/en
Application filed by Dow Chemical Co filed Critical Dow Chemical Co
Priority to EP87103843A priority patent/EP0282614A1/fr
Publication of EP0282614A1 publication Critical patent/EP0282614A1/fr
Withdrawn legal-status Critical Current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
    • C25B9/60—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
    • C25B9/70—Assemblies comprising two or more cells
    • C25B9/73—Assemblies comprising two or more cells of the filter-press type
    • C25B9/77—Assemblies comprising two or more cells of the filter-press type having diaphragms

Definitions

  • This invention relates to an electrochemical cell and in particular to a structural frame for use in an electrochemical cell.
  • alkali metal chlorates such as sodium chlorate
  • sodium chlorate have been formed electrolytically from a sodium chloride brine in cells without a separator positioned between the anode and the cathode.
  • the electrolytic products will normally be gaseous chlorine, hydrogen gas, and an aqueous solution containing sodium hydroxide.
  • the newer, so-called flat plate electrochemical cells using a planar piece of ion exchange membrane to separate the anolyte from the catholyte compartments also have a plurality of solid, liquid impervious frames adapted to support the anode on one side and the cathode on the opposite side.
  • These frames have previously been constructed of materials such as metal and plastic, but neither of these materials has been found to be entirely satisfactory.
  • electrolyte may leak from within the cell to the exterior.
  • plastic frames are not generally subject to the electro-lytic attack, but are normally not resistant to the anolyte and/or catholyte within the cell under operating conditions for extended periods of time, for example, several years.
  • the present invention particularly resides in a structural frame adapted for use in an electrochemical cell comprising: a central cell element in the form of a generally planar member made of a polymeric material having a plurality or horizontally and vertically spaced-apart shoulders protruding outwardly from at least one surface of said planar member; at least one electrically conductive insert extending from an exterior face of a shoulder on one surface of the planar member, through the planar member, to an exterior face of a shoulder on the opposite surface of the planar member, wherein each of said shoulders annularly encircles and supports each of said inserts, an electrically conductive, substantially completely hydraulically impermeable liner cover resistant to the corrosive effects of an electrolyte in said cell matingly contacted with at least one of said surfaces of said planar member and adapted to minimize contact between the electrolyte in said cell and said planar member.
  • an anolyte cover is matingly affixed to the anolyte surface of the planar member and adapted to minimize contact between the anolyte and the planar member.
  • the anolyte cover is resistant to the corrosive effects of the anolyte.
  • a catholyte cover is matingly affixed to the opposite, catholyte surface of the planar member and adapted to minimize contact between the catholyte and the planar member.
  • the catholyte cover is resistant to the corrosive effects of the catholyte.
  • Both the anolyte cover and the catholyte cover may be made from a metal or, from another material which is provided with metallic inserts molded into the non-metallic liner at the points where the metallic inserts in the liner contact the metallic inserts which pass through the planar member.
  • the invention further includes an electro­chemical cell utilizing a plurality of the above described structural frames removably and sealably positioned in a generally coplanar relationship with each other and with each of the planar members being spaced apart by an anode on one or opposite sides of the planar member and a cathode on an opposing side of the planar memberor by an anode on one side and a cathode on the opposite side of the planar member.
  • Figure 1 In Figure 1 are shown structural frames 10 and 10a, which achieve the above objects. It is illustrated for use in an electrochemical cell for producing gaseous chlorine in aqueous alkali metal hydroxide solution.
  • the present invention can be beneficially employed to produce chlorine and various alkali metal hydroxide solutions, it is preferred to use sodium chloride as the primary salt in the starting brine since this particular salt is readily available commercially and there are many well established uses for sodium hydroxide produced electrolytically.
  • the cell structure 10 includes a generally planar member 12 comprising a planar barrier portion, a peripheral flange portion (34), and anode and cathode standoff means or bosses for maintaining the anode and cathode of adjacent cell structures at a predetermined distance from the planar barrier portion.
  • the planar member can be produced by commercial and known procedures into a shape with a plurality or hori­zontally and vertically spaced apart shoulders 14 and 14a (bosses) protruding outwardly from cathode and anode sides 16 and 18, respectively.
  • the peripheral surface 20 of the planar member 12 defines the outer surface of the electrochemical cell when a plurality of the planar members are positioned together as shown in the drawing.
  • the peripheral configuration of the planar members 12 is optional and can be varied to suit the particular configuration of the electrochemical cell shape desired.
  • the number, size, and shape of the shoulders 14 and 14a may be an important consideration in both the design and operation of the present invention. They may be square, rectangular, conical, cylindrical, or any other convenient shape when viewed in sections taken either parallel or perpendicular to the central portion.
  • the shoulders may have an elongated shape to form a series of spaced ribs distributed over the surface of the plastic member.
  • a number of polymeric materials are suitable for use in the present invention for the construction of the planar member.
  • suitable materials include polyethylene; polypropylene; polyvinylchloride; chlorinated polyvinyl chloride; acrylonitrile, polystyrene, polysulfone, styrene acrylonitrile, butadiene and styrene copolymers; epoxy; vinyl esters; polyesters; and fluoroplastics and copolymers thereof.
  • a polymeric material such as polypropylene be used for the planar member since it produces a shape with adequate structural integrity at elevated temperatures, is readily available, and is relatively inexpensive with respect to other suitable materials.
  • planar member 12 can be produced by any of a number of processes known well to those skilled in the art of plastic molding. Such molding processes include, for example, injection molding, compression molding, transfer molding, and casting. Of these processes, injection molding has been found to satisfactorily produce a structure with adequate strength for use in an electrochemical cell.
  • the polymeric material is injected into a mold containing the desired number of inserts (dis­cussed later). In this manner, the planar member is a one-piece member which fits tightly around the inserts holds them in place, and provides a high degree of support to them. Such a configuration minimizes the likelihood that the inserts will separate from the planar member and become loose.
  • planar member 12 When the planar member 12 is employed in an electrochemical cell for producing chlorine, the temperature of the cell and the planar member will frequently reach, or be maintained at, temperatures of from 60° to 90°C. At these temperatures polymeric materials, as do most materials, expand a measurable amount. Any expansion and later contraction on cooling of the planar member could result in electrolyte seeping from within the plurality of cells when joined together or, more importantly, could result in distor­tion of the anode and cathode which are made of metallic expanded mesh or perforated sheets. Furthermore, the differential expansion between the planar member 12 an electrolyte linear or cover 22 and/or 24 would create stress on the welds which affix these covers to the inserts which are themselves molded in the planar member.
  • an additive to reduce thermally induce expansion of the planar member. More preferably, the additive will also increase the structural strength of the finished article.
  • Such additive can be, for example, fiberglass, graphite fibers, carbon fibers, talc, glass beads, pulverized mica, asbestos, and the like, and combinations thereof.
  • the polymer contain from 5 to 75 weight percent and more preferably from 10 to 40 weight percent of the additive. Glass fibers can be readily mixed with polypropylene to produce an injectable material suitable for use in the present invention which results in a solid, physically strong body with a coefficient of expansion less than polypropylene not containing glass fibers. Of greater importance is the need to minimize the difference in expansion between the planar member, the electrodes, and the current collector, since these elements are welded together and it is critical that they remain substantially flat and parallel.
  • At least one electric conducting element such as insert(s) 26, is positioned and preferably molded into the planar member 12.
  • the insert(s) 26 extends through the planar member from one electrolyte surface, e.g. the catholyte surface 16 to an opposite electrolyte surface, e.g. the anolyte surface 18.
  • the inserts 26 and 26a are preferably retained within the planar member 12 by means of friction between the polymeric material and the insert. It is more preferable to increase the friction between these two bodies by having an additional means to restrain the insert within the polymeric material.
  • Such additional means include, for example grooves (one or more) around the circumference of the insert(s), keys welded to the insert, hole(s) extending into and/or through the insert, slots, rings, collars, studs, or bosses.
  • the insert(s) 26 can be any material which will permit flow of an electric current between the catholyte cover 22 and the anolyte cover 24. Since the covers 22 and 24 are preferably made of a metal, it is convenient to fabricate the insert from a metal, such as aluminum, copper, iron, steel, nickel, titanium, and the like, or alloys or physical combinations including such metals.
  • the shoulders and inserts should be spaced so that they provide a somewhat uniform and low electrical potential gradient across the face of the electrode to which they are attached. They should be spaced so that they allow free fluid circulation from any unoccupied point within their respective electrolyte compartment to any other unoccupied point within that compartment. Thus the shoulders will be somewhat uniformly spaced apart from one another in their respective compartments.
  • the insert 26 is preferably made of a material weldably compatible with the particular cover it contacts.
  • the insert 26 may be a welded assembly of a steel rod 261 with a vanadium disk 262 interposed between and welded to both the rod 261 and a titanium cup-like member 263 on the anode facing portion of the structure 10.
  • a similar nickel cup-like member 264 may be welded directly to the rod 261 on the cathode facing portion of the insert.
  • the titanium and nickel members 263 and 264, respectively, are then readily weldable to the titanium anolyte cover 24 and the nickel catholyte cover 22 and 22a preferred for use in an electrochemical cell producing chlorine and an aqueous sodium hydroxide solution.
  • both the anolyte and the catholyte covers are so shaped to correspond closely to the exterior surface of the planar member 12. In some instances, the covers 22 or 24 may abut the frame 10 in one or more locations.
  • both the covers 22 and 24 which are exposed to the anolyte or catholyte and span the planar member contain no openings through which electrolyte or electrolytic products can pass during operation of the electrochemical cell.
  • the freedom from openings through the covers minimizes the likelihood that electrolyte will leak or seep through holes or spaces around gaskets of other seals and come into contact with the planar member.
  • the anolyte cover 24 is made of a material which is resistant to the anolyte during operation of the cell. Normally, this material is not electrolytically active, but the invention is still operable if the material does become or is active electrolytically. Suitable materials are, for example, titanium, tantalum, zirconium, tungsten, and other valve metals not materially affected by the anolyte. Titanium is preferred as the anolyte cover.
  • the catholyte cover 22 is resistant to attack by the catholyte under the conditions present in the electrochemical cell.
  • Suitable materials for the catholyte cover include, for example, iron, steel, stainless steel, nickel, lead, molybdenum, and cobalt and alloys, including major portions of these metals.
  • Nickel, including nickel base alloys, is preferably used for the catholyte cover, since nickel and nickel alloys are generally resistant to the corrosive effects of the catholyte, especially an aqueous catholyte solution containing up to at least about 35 weight percent sodium hydroxide.
  • Steel has also been found to be suitable, and relatively inexpensive, for use in a cell as a catholyte cover in the presence of a dilute (i.e., up to about 22 weight percent) aqueous solution of sodium hydroxide.
  • flanges 34 and 34a extending outwardly from the main structural portion of the planar member 12 along the periphery of the planar member.
  • the flanges extend outwardly from the planar member about the same distance as the insert 26.
  • separate spacer elements could be utilized to build up to the planar member 12 sufficiently to permit a number of the planar members to be combined into a cell series without having electrolyte, either anolyte or catholyte, leak from within the catholyte and anolyte compartments 30 and 32, respectively, to an exterior portion of the cell.
  • FIG. 1 further shows an anode 36 which is positively charged during operation of the cell from an external power source (not shown), electrically connected to the anolyte cover 24.
  • anode 36 which is positively charged during operation of the cell from an external power source (not shown), electrically connected to the anolyte cover 24.
  • Such electrical connection is readily achieved by welding the anode 36 to the anode cover where the anode cover comes into physical contact with the insert 26.
  • the anolyte cover 24 is welded to the insert 26 and the anode 36 is welded to the anolyte cover 24 adjacent to the insert 26.
  • Various means of welding can be utilized in the present invention, but it has been found highly satisfactory to use resistance or capacitance discharge welding techniques.
  • the anode 36 can additionally be welded to the cover 24 at anode end portion 42 by, for example, resistance or capacitance discharge welding.
  • Other suitable welding techniques include tungsten inert gas (TIG) and metal inert gas (MIG) welding.
  • the anode 36 is a metal, such as one of the common film-forming metals, which is resistant to the corrosive effects of the anolyte during the operation of the cell.
  • Suitable metals are well known to include tantalum, tungsten, columbium, zirconium, molybdenum, and preferably, titanium and alloys containing major amounts of these metals, coated with an activating substance, for example, an oxide of a platinum group metals, such as ruthenium, iridium, rhodium, platinum, palladium, either alone or in combination with an oxide of a film-forming metal.
  • an activating substance for example, an oxide of a platinum group metals, such as ruthenium, iridium, rhodium, platinum, palladium, either alone or in combination with an oxide of a film-forming metal.
  • Other suitable activating oxides include cobalt oxide either along or in combination with other metal oxides. Examples of such activating oxides are found in U.S.
  • the cathode 38 and 38a which has a negative electric potential during operation of the cell, is electrically connected to the catholyte cover 22 and 22a, respectively, in substantially the same manner as above described for the anode 36.
  • the cathode 38 and 38a should be constructed of a material which is resistant to the corrosive effects of the catholyte during operation of the cell. Materials suitable for contact with the catholyte will depend upon the concentration of the alkali metal hydroxide in the aqueous solution and may be readily determined by one skilled in the art.
  • cathode materials such as iron, nickel, lead, molybdenum, cobalt, and alloys including major amounts of these metals, such as low carbon stainless steel, are suitable for use as the cathode.
  • the cathodic electrodes may optionally be coated with an activating substance to improve perfor­mance of the cell.
  • a nickel substrate could be coated with oxides of nickel and a platinum group metal, such as, ruthenium, or nickel and a platinum group metal, or oxide thereof such as ruthenium oxide, to reduce hydrogen overvoltage.
  • ruthenium or nickel and a platinum group metal, or oxide thereof such as ruthenium oxide
  • both the anode and the cathode are permeable to the respective electrolyte.
  • the electrodes can be made permeable by several means including, for example, using a punched sheet or plate, an expanded mesh, or woven wire.
  • the anode should be sufficiently porous to permit anolyte and chlorine to pass therethrough and the cathode should be sufficiently porous to permit catholyte to pass therethrough and hydrogen to pass therethrough.
  • the electrochemical cell of Figure 1 also shows the anode 36 and the cathode 38 spaced apart by an ion exchange membrane 44 which is in contact with the anode 36. If desired, however, although not preferred, the membrane 44 could be in contact with the cathode 38 or be suspended between the two electrodes. It is important, that the ion exchange membrane 44 separate the anode compartment 32 from the cathode compartment 30a.
  • At least one gasket 46 is positioned between the frames 10 and 10a.
  • a compressive force is applied to the extremes of the frames to compress the gasket material 46 so that it both seals the ion exchange membrane 44 in position and minimizes leakage of electrolyte from within the final cell series to the exterior of the cells.
  • the membrane 44 is positioned to substantially entirely prevent leakage of electrolyte from within the final cell series to the exterior of the cells.
  • gaskets materials can be used including, for example, fluorocarbon, chlorinated polyethylene rubber, and ethylene propylene diene terpolymer rubber.
  • Figure 2 is an exploded, partially cross­sectioned isometric view of the structural frame 10b, including a planar member 12a with a plurality of frustoconical shoulders 14b, with inserts 26a encased therein, extending outwardly from the generally planar anolyte surface 18a.
  • Identical shoulders 14c extend outwardly from the catholyte surface of the planar member 12a in a mirror image relationship with the shoulders 14b on the anolyte surface.
  • a conduit or opening 48 is provided in the planar member 12a to permit exit of production produced in the electrochemical cell during operation.
  • a pipe, tube, or shaped metal conduit is positioned within the opening 48 and affixed to the cover 24b to facilitate substantially leak free removal of the product from the cell.
  • a similar opening and conduit (not shown) is provided in, for example, a wall portion of the planar member at a location generally diagonally opposed to the opening 48 to permit an aqueous sodium chloride solution to be fed through the conduit into the anode compartment.
  • Similar openings and conduits are provided on the cathode side of the planar member to permit feeding, for example, water into the cathode compartment and removal of products, such as a solution containing sodium hydroxide, and optionally hydrogen, therefrom.
  • the anolyte cover 24b and catholyte cover 22a are adapted to closely fit over the respective surface of the planar member 12a and prevent entrance of electrolyte from the respective electrode compartments into the space, if any, between the cover and the planar member.
  • the covers 22a and 24b also have conduits therein for exit of the brine solution and product produced in the respective electrolyte compartment and feeding of starting solutions to the respective compartments.
  • a shaped pipe 50, in the cover 24b corresponds to the opening 48 in the planar member to afford ready exit of the product chlorine and spent anolyte from the anode compartment.
  • An expanded mesh anode 36b and an expanded mesh cathode 38a are adapted to fit within the respective anolyte and catholyte covers substantially the same as shown in Figure 1.
  • An ion exchange membrane is shown in sheet 44a.
  • a leak minimizing gasketing material 46a is placed between structural frame members prior to the assembly of an electrochemical cell series.
  • Figure 3 is shown a partially assembled cell series containing three sets of structural frame members with anodes and cathodes spaced apart by ion exchange membranes as shown in the previous figures.
  • the inserts 26b, 26c, 26d, and 26e are of different configurations than those shown in Figures 1 and 2.
  • the insert 26d is a tubular member with a roughened exterior surface and an electrically conducting end portion 52 physically and electrically connected to end covering the entire cross-section of the tubular insert 26d.
  • Such electrical and physically connection can be obtained by welding or other known bonding techniques as known to those skilled in the particular art.
  • the peripheral portions of the cover 24b may optionally contain expansion grooves (not shown) to minimize any effects of thermal expansion of the covers upon the operation of the cell.
  • a pH of from about 0.5 to about 5.0 is desired to be maintained.
  • the feed brine preferably contains only minor amounts of multivalent cations (less than about 80 parts per billion when expressed as calcium). More multivalent cation concentration is tolerated with the same beneficial results if the feed brine contains carbon dioxide in concentrations lower then about 70 ppm when the pH of the feed brine is lower than 3.5.
  • Operating temperatures range from 0° to 110°C, preferably from 60°C to 80°C.
  • Brine purified from multivalent cations by ion-exchange resins after conventional brine treatment has occurred is particularly useful in prolonging the life of the membrane.
  • a low iron content in the feed brine is desired to prolong the life of the membrane.
  • the pH of the brine feed is maintained at a pH below 4.0 by the addition of hydrochloric acid.
  • the operating pressure is maintained at less than 7 atmospheres.
  • the cell is operated at a current density of from 1.0 to 4.0 amperes per square inch, but in some cases operating above 4.0 amps/in.2 is quite acceptable.

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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)
EP87103843A 1985-12-16 1987-03-17 Cadre de construction pour une cellule électrochimique Withdrawn EP0282614A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
US06/809,372 US4666580A (en) 1985-12-16 1985-12-16 Structural frame for an electrochemical cell
EP87103843A EP0282614A1 (fr) 1987-03-17 1987-03-17 Cadre de construction pour une cellule électrochimique

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
EP87103843A EP0282614A1 (fr) 1987-03-17 1987-03-17 Cadre de construction pour une cellule électrochimique

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EP0282614A1 true EP0282614A1 (fr) 1988-09-21

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EP87103843A Withdrawn EP0282614A1 (fr) 1985-12-16 1987-03-17 Cadre de construction pour une cellule électrochimique

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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2647468A1 (fr) * 1989-05-29 1990-11-30 Solvay Chassis pour electrolyseur du type filtre-presse et electrolyseurs du type filtre-presse

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2600345A1 (de) * 1976-01-07 1977-07-21 H T Hydrotechnik Gmbh Nach art von filterpressen gebauter elektrolyseapparat
EP0185270A1 (fr) * 1984-12-17 1986-06-25 The Dow Chemical Company Procédé de fabrication d'un élément unitaire de transmission de courant électrique pour un assemblage de cellules électrochimiques du type filtre-presse monopolaire ou bipolaire
US4666580A (en) * 1985-12-16 1987-05-19 The Dow Chemical Company Structural frame for an electrochemical cell

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2600345A1 (de) * 1976-01-07 1977-07-21 H T Hydrotechnik Gmbh Nach art von filterpressen gebauter elektrolyseapparat
EP0185270A1 (fr) * 1984-12-17 1986-06-25 The Dow Chemical Company Procédé de fabrication d'un élément unitaire de transmission de courant électrique pour un assemblage de cellules électrochimiques du type filtre-presse monopolaire ou bipolaire
US4666580A (en) * 1985-12-16 1987-05-19 The Dow Chemical Company Structural frame for an electrochemical cell

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
FR2647468A1 (fr) * 1989-05-29 1990-11-30 Solvay Chassis pour electrolyseur du type filtre-presse et electrolyseurs du type filtre-presse
EP0400712A1 (fr) * 1989-05-29 1990-12-05 SOLVAY (Société Anonyme) Châssis pour électrolyseur du type filtre-presse et électrolyseurs du type filtre-presse

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