CN101370966A - Elastic current distributor for percolating cells - Google Patents

Elastic current distributor for percolating cells Download PDF

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Publication number
CN101370966A
CN101370966A CNA2007800024095A CN200780002409A CN101370966A CN 101370966 A CN101370966 A CN 101370966A CN A2007800024095 A CNA2007800024095 A CN A2007800024095A CN 200780002409 A CN200780002409 A CN 200780002409A CN 101370966 A CN101370966 A CN 101370966A
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Prior art keywords
electrolyzer
diffusion electrode
gas diffusion
tinsel
conductive protrusions
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CNA2007800024095A
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Chinese (zh)
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CN101370966B (en
Inventor
F·费德里科
P·沃尔特林
L·卡勒廷
D·欧达尼
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ThyssenKrupp Uhde Chlorine Engineers Italia SRL
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Uhdenora SpA
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8605—Porous electrodes
    • 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
    • C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
    • C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
    • C25B11/03—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form perforated or foraminous
    • 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
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
    • H01M8/023—Porous and characterised by the material
    • H01M8/0232—Metals or alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Abstract

Described is a membrane electrolysis cell comprising an anodic compartment and a cathodic compartment, wherein at least one of the two compartments contains a gas- diffusion electrode, and a planar porous element traversed by an electrolyte flow is interposed between membrane and gas-diffusion electrode. The electric current transmission to the gas-diffusion electrode is effected through a current distributor provided with elastic conductive protrusions pushing the electrode against the porous element.

Description

The elasticity distributing switch that is used for the diafiltration electrolyzer
Technical field
The present invention relates to be used for the electrolyzer of industrial electrolysis process, and be particularly related to the electrolyzer that comprises by separated anodal compartment of ion-exchange membrane and cathodic compartment, one of them or two compartments are equipped with gas diffusion electrode and technology electrolytic solution to flow through the multihole device of percolator or equivalence.
Background technology
In the following description, to mention and be applicable to the electrolytic electrolyzer of unpolarized chloro-alkali, be the electrolytic process of alkali metal chloride brines, thereby wherein hydrogen evolution cathodic reaction is suppressed the reaction of oxygen consumption that helps on the gas diffusion cathode, for example EP1033419 is disclosed; Yet the present invention is not limited to chloro-alkali electrolyzer, and it can be used for the electrochemistry in industry process of any employing gas diffusion electrode.
The depolarize chloro-alkali electrolyzer of special advanced type is known in the art, and wherein technology electrolytic solution flows through suitable porous plane component or percolator under action of gravity: for example disclose such electrolyzer among the WO/0157290.In such electrolyzer, typically there is the anodal compartment that obtains by the titanium housing, wherein supply the strong brine of alkali metal chloride and comprise and have the titanium anode of analysing the chlorine catalyst coatings, and cathodic compartment is limited by the nickel cathode housing; These two compartments are separated by cationic exchange membrane.The caustic soda that produces in technology passes the multihole device that is inserted in the cathodic compartment because of gravity flowage, and described multihole device one side contacts with ion-exchange membrane, and opposite side contacts with gas diffusion cathode.In other words, when anode is by being selected from that suitable metal construction well known in the art (for example rib array) is electrically connected with anode casing and during the rigid metal element of mechanical connection, negative electrode is the thin multihole device that the non-self-supporting equivalent structure by silver-colored net, carbon cloth or other type obtains.Therefore, the current delivery from the rear wall of anode casing to gas diffusion electrode must be affected because of bigger displacement contact and structure that can the mechanical support electrode are provided.For improving electrochemical properties, also must (for example 0.1 arrive 0.5kg/cm with specified pressure 2) negative electrode is pushed into percolator, so that when helping restriction round-robin liquid electrolyte, allow electric continuity.For satisfying all above-mentioned conditions, the electrolyzer of prior art has the electric current feed system that depends on two kinds of different elements: the first, constitute the rigid current collector of a cathode shell part, and it can be made of for example rib array, as in anode side; The second, the wire cloth between rigid current collector and gas diffusion electrode, under suitable contractive condition, this wire cloth can guarantee enough pressure transmission to gas diffusion electrode the electric continuity expected thus.Equivalent processes is used to improve traditional chloro-alkali electrolyzer, so that it is applicable to the percolation type process of depolarization, for example Fig. 2 of WO 03/102271 is illustrated: in this case, initial electric tank cathode serves as collector, nickel wire net (elastic collector) serves as the intermediary element of the current delivery between rigid current collector and the gas diffusion electrode simultaneously, and described initial electrolysis groove negative electrode is the metal electrode of being made by nickel or steel that is used for liberation of hydrogen as known in the art.
Yet, aforesaid method also can bring some inconvenience, hindered the commercialization of this type electrolyzer: two element type current transmission system in fact related to expensive and thickness, difficulty and silk screen (particularly peripheral region) size control difficulty were installed, were difficult to controlled deformation and elastic force, thereby also exist the increase contact interface not to be particularly conducive to ohmic voltage drop in addition certainly, for example the interface between silk screen and the gas diffusion electrode.
Summary of the invention
An object of the present invention is to provide and separated by ion-exchange membrane and be equipped with the diafiltration element that is used for circulation of elecrolyte and the electrolyzer of gas diffusion electrode, overcome the limitation of prior art.
On the other hand, an object of the present invention is to provide the improvement electric current feed system that is used for electrolyzer, this electrolyzer has gas diffusion electrode and percolator.
The present invention is made up of the electrolyzer that has by separated anodal compartment of ion-exchange membrane and cathodic compartment, wherein said two compartments are equipped with one of at least the gas diffusion electrode with two interareas, first interarea towards film contacts with the percolator that is passed by electrolyte stream, second interarea relative with first interarea contacts with distributing switch, and this distributing switch comprises and is applicable to a plurality of elastic conductive thrusts of gas diffusion electrode being pressed to percolator.Disclosed as WO/0157290, as percolator, expectation is suitable for any porous plane component that liquid flow is passed under action of gravity.In a preferred embodiment, the distributing switch that cutting and the moulding by single tinsel obtained to replace rigid current collector of the prior art-elastic collector assembly, for example the nickel sheet in the cathode current collector situation of chloro-alkali electrolyzer.In this case, the nickel sheet is that thickness is typically 0.5 to 1.5mm sheet, preferably has the coating that is suitable for reducing contact resistance.The nickel material of this sheet can be an alloying differently, for example is selected from the classification of common obtainable product; Selection has and is applicable to that the grade of making spring and the nickel material of mechanical property (for example having excellent elasticity) will prove particularly advantageous.In a simple especially and effective embodiment, the conductive protrusions that can apply enough pressure to electrode is the spring joint of arranging in pairs (tag), makes two adjacent spring joints from the interarea of the tinsel that they derived from projection round about.Obtained the more effective and uniform support in entire electrode surface by this way.Such scheme is applicable to the almost best design of electrolysis cells of every kind of processing condition; Yet, use has the advantage that allows effective gas circulation (the electrolytic situation of depolarize chloro-alkali for example according to the silk screen of prior art as the contact member under the high current density, with oxygen effective supply gas diffusion electrode), and this possibly can't have simple sheet structure.In this case, particularly preferred embodiment provides the conductive protrusions of single watt of (tile) form, and they comprise successively and one or morely are used to provide the spring joint that electrically contacts and one or morely are convenient to the opening that gas passes through.Conductive protrusions can be for example with the parallel columns setting along the entire electrode surface arrangement.
Be suitable for preferred 0.1 to 0.5kg/cm according to distributing switch of the present invention 2Pressure under directly on the gas diffusion electrode surface, realize effectively electrically contacting, therefore need not contact interface (in the prior art, rigid current collector is coupled with elastic collector) about prior art systems; On the other hand, in one embodiment of the invention, can distribute the add ons of mechanical compression force to be inserted between distributing switch and the gas diffusion electrode with being used to, this add ons be made of for example thin net or porous chips or punched sheet.In this case, the number of contact interface and prior art quite, yet corresponding resistance significantly is lower than and makes the almost nonelastic silk screen of prior art directly contact the resistance that is obtained with gas diffusion electrode.In addition, those skilled in the art will readily understand that the total thickness of electrolyzer is significantly lower.
Description of drawings:
To more at large describe the present invention by accompanying drawing, these accompanying drawings only limit to give an example purpose and are not intended to limit the present invention.
-Fig. 1 has shown the percolation type depolarize chloro-alkali electrolyzer according to prior art.
-Fig. 2 has shown according to percolation type depolarize chloro-alkali electrolyzer of the present invention.
-Fig. 3 has shown first embodiment according to distributing switch of the present invention.
-Fig. 4 has shown second embodiment according to distributing switch of the present invention.
-Fig. 5 has shown the 3rd embodiment according to distributing switch of the present invention.
Embodiment
Fig. 1 has shown the percolation type depolarize chloro-alkali electrolyzer according to prior art, and it comprises by the separated anodal compartment of ion-exchange membrane (500) and a cathodic compartment.Cathodic compartment is limited by cathodic back-wall (101), contacts with the electric current feed system that depends on two kinds of different elements, and rigid current collector (201) constitutes its part, and the silk screen that elastic collector (210) is made by for example nickel constitutes.Negative electrode (301) is made of the porous gas diffusive electrode for aerobic, and a side contacts with silk screen (210), and opposite side contacts with the percolator (400) that the plane multihole device that is passed by electrolyte stream under action of gravity constitutes.The ion-exchange membrane (500) that serves as spacer body has the cathode plane that contacts with percolator (400) and towards the anode surface of anode (302), this anode surface can be in contact with it or keep little predetermined distance.Anode (302) comprises the titanium-base that is made of net or porous chips or punched sheet usually, or optional by two stacked titanium-bases that constitute of such element; Anode substrate has the catalyst coatings that chlorine is separated out that is used for commonly known in the art.Electric continuity between anode (302) and the anodal compartment rear wall (102) is guaranteed by rigid current collector (202).Negative electrode (201) rigid current collector and anode (202) rigid current collector can by rib array, beading, have appropriate intervals hole (gopher) sheet or well known to a person skilled in the art that the collector of other type constitutes.Fig. 2 has shown according to percolation type depolarize chloro-alkali of the present invention, wherein adopts identical reference number mark with the electrolyzer components identical of Fig. 1.
Electric current feed system is made of a plurality of conductive protrusions (220), for example is applicable to gas diffusion electrode (301) is pressed to the spring of percolator (400) or the assembly of elastomeric spring joint; Between conductive protrusions (220) assembly and gas diffusion electrode (301), insert the selectable unit (230) that distributes mechanical compression force, for example thin net or porous chips or punched sheet.
Fig. 3 has shown an embodiment of a plurality of conductive protrusions that obtained by single tinsel, and the assembly of the elastomeric spring joint (221) that is arranged in parallel for how much by the foundation pectination in this situation constitutes: spring joint is arranged in pairs, makes per two spring joints outstanding in the opposite direction from the interarea of initial tinsel.According to the size of electrolyzer, the single row of spring joint (221) can cover whole active surface, maybe can be arranged side by side more row, as those skilled in the art know.
Fig. 4 has shown the preferred embodiment of a plurality of conductive protrusions that obtained by single tinsel: thrust preferably passes through the cutting of sheet and single watt on the tetragon (222) that moulding obtains in this case, optional being welded direct on the rigid current collector (201), in them each all comprises the element with difference in functionality: for example, by suitable folding step, each watt acquisition has the edge (223) of about 90 ° of bending angle, so that give the rigidity that needs.The spring joint that a plurality of appropriate intervals are opened (224) serves as the contact member with gas diffusion electrode (301), and a plurality of holes (225) help the supply and the circulation of gas, is meant the oxygen that cathodic reaction needs in this case especially.The difference that is welded to rigid current collector (201) watt preferably is arranged in the parallel columns of optional skew.
Fig. 5 has shown the variant of the preferred embodiment of a plurality of conductive protrusions that obtained by single tinsel shown in Fig. 4: initial in this case tinsel is a punched sheet, and extend on the entire body of watt (222) that comprise spring joint (224) a plurality of holes (225 ').Obtain enhanced gas by this way and supply with, when spring joint (224) be compressed and in the place of their projections when described contacts this supply effectively finish up to stroke.Also obtain a small amount of the saving during making, the independent execution in the hole (225) shown in being gone up by watt (222) among Fig. 4 constitutes.Watt structure further mechanics advantage also is provided: in unexpected high negative electrode counterpressure situation (for example because of the mistake of processing condition control, perhaps because of the error of element operation or assembling), since GDE whole watt lip-deep near, tension set does not take place in spring joint.In this case, it will be apparent to those skilled in the art that obtaining these watts by punched sheet is more importantly for guaranteeing that under any circumstance correct gas is supplied with.
Embodiment 1
According to the design among Fig. 2, for having 0.16m 2Following element is assembled with the experiment electrolyzer in the laboratory of useful area: the titanium that possesses ruthenium and titanium oxide base catalyst coatings
Figure A200780002409D00081
Anode (302), by Dupont/USA supply N982 ion-exchange membrane (500), nickel foam percolator, by the gas diffusion electrode that constitutes by argentum-based catalyzer activatory silver net.
Electric current feed system comprises a plurality of elastic conductive thrusts, and each described thrust is made of as shown in Figure 5 watt (222) that the thick nickel punched sheet of 1mm obtains.
At 4kA/m 2Current density and 90 ℃ temperature under, be the circulation sodium chloride brine of 210g/1 to anode electrolytic cell compartment feed consistency.Cathode product is made of the caustic soda of the 32 weight % that are downward through percolator.Under these conditions, the stable process conditions on the equipment after 10 days, is detected 2.00 to 2.05V bath voltage.
Embodiment 2
Under simulated condition, utilize the test of the electrolyzer repetition embodiment 1 of prior art.Therefore, significantly difference only is the cathodic current feeder system, and it comprises the rigid current collector structure that is made of the nickel rib array, and described nickel rib array is welded to and commercial nickel screen bonded cathodic back-wall.
Under the processing condition identical, after 10 days, detect 2.10 to 2.15V bath voltage in stabilization with embodiment 1.
The description of front is not intended to limit the present invention, can use the present invention and not deviate from scope of the present invention according to different embodiments, and scope of the present invention only is defined by the following claims.
In the application's specification sheets and claim, term " comprises " and variant is not intended to get rid of other key element or accrete existence as " comprising ", " containing ".

Claims (12)

1. electrolyzer, its type is the electrolyzer that comprises by separated anodal compartment of ion-exchange membrane and cathodic compartment, at least one of described compartment is equipped with the gas diffusion electrode with two interareas, first interarea of described gas diffusion electrode towards described film and be suitable for the plane multihole device that electrolyte stream passes and contact, second interarea of described gas diffusion electrode contacts with distributing switch, and this distributing switch comprises a plurality of elastic conductive thrusts that are suitable for described gas diffusion electrode is pressed to described plane multihole device.
2. the electrolyzer of claim 1, wherein said a plurality of conductive protrusions apply 0.1 to 0.5kg/cm on gas diffusion electrode 2Pressure.
3. claim 1 or 2 electrolyzer, the described distributing switch that wherein comprises described a plurality of conductive protrusions is to obtain by the cutting of tinsel and moulding.
4. the electrolyzer of claim 3, wherein said a plurality of conductive protrusions are the spring joints according to the pectination geometry arrangement.
5. the electrolyzer of claim 4, wherein said spring joint is arranged with the phase adjacency pair, and the spring joint of each described centering is outstanding in the opposite direction from the interarea of described tinsel.
6. the electrolyzer of claim 3, wherein said conductive protrusions is to be chosen as tetragonal independent watt, described watt comprises a plurality of spring joints and at least one is used for the opening of gas circulation.
7. the electrolyzer of claim 6, wherein said watt is welded to rigid current collector with optional offset collimated row.
8. each electrolyzer in the claim 3 to 7, wherein said tinsel has 0.5 to 1.5 millimeter thickness.
9. each electrolyzer in the claim 3 to 6, wherein said tinsel is a punched sheet.
10. each electrolyzer in the claim 3 to 9, wherein said tinsel is made by nickel.
11. the electrolyzer of claim 10, wherein said nickel sheet has the coating that is suitable for reducing the contact resistance relevant with described thrust.
12. each electrolyzer of aforementioned claim, it comprises the add ons that is used to distribute mechanical compression force that is inserted between described distributing switch and the described gas diffusion electrode, and described add ons is selected from net, punched sheet and porous chips.
CN2007800024095A 2006-01-16 2007-01-15 Elastic current distributor for percolating cells Expired - Fee Related CN101370966B (en)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
ITMI2006A000054 2006-01-16
IT000054A ITMI20060054A1 (en) 2006-01-16 2006-01-16 ELASTIC CURRENT DISTRIBUTOR FOR PERCOLATOR CELLS
PCT/EP2007/050362 WO2007080193A2 (en) 2006-01-16 2007-01-15 Elastic current distributor for percolating cells

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CN101370966A true CN101370966A (en) 2009-02-18
CN101370966B CN101370966B (en) 2013-05-08

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CN106460203A (en) * 2014-06-24 2017-02-22 凯密迪公司 Narrow gap, undivided electrolysis cell
CN109312477A (en) * 2016-06-14 2019-02-05 蒂森克虏伯伍德氯工程有限公司 Electrolytic cell including elastic component
CN112262231A (en) * 2018-06-14 2021-01-22 蒂森克虏伯伍德氯工程有限公司 Electrolytic cell with elastic retaining element

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CN106460203A (en) * 2014-06-24 2017-02-22 凯密迪公司 Narrow gap, undivided electrolysis cell
CN109312477A (en) * 2016-06-14 2019-02-05 蒂森克虏伯伍德氯工程有限公司 Electrolytic cell including elastic component
CN112262231A (en) * 2018-06-14 2021-01-22 蒂森克虏伯伍德氯工程有限公司 Electrolytic cell with elastic retaining element
CN112262231B (en) * 2018-06-14 2023-09-05 蒂森克虏伯伍德氯工程有限公司 Electrolytic cell with elastic holding element

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WO2007080193A2 (en) 2007-07-19
JP5860075B2 (en) 2016-02-16
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