CN101370966B - Elastic current distributor for percolating cells - Google Patents

Elastic current distributor for percolating cells Download PDF

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Publication number
CN101370966B
CN101370966B CN2007800024095A CN200780002409A CN101370966B CN 101370966 B CN101370966 B CN 101370966B CN 2007800024095 A CN2007800024095 A CN 2007800024095A CN 200780002409 A CN200780002409 A CN 200780002409A CN 101370966 B CN101370966 B CN 101370966B
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electrolyzer
diffusion electrode
gas diffusion
tinsel
watt
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CN101370966A (en
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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

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
  • Electrodes For Compound Or Non-Metal Manufacture (AREA)
  • Fuel Cell (AREA)
  • Micro-Organisms Or Cultivation Processes Thereof (AREA)

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 the electrolyzer for the industrial electrolysis process, and be particularly related to the electrolyzer that comprises by the separated anodal compartment of ion-exchange membrane and cathodic compartment, wherein one or two compartment is equipped with gas diffusion electrode and technique electrolytic solution to flow through the multihole device of percolator or equivalence.
Background technology
In the following description, the electrolyzer that is applicable to the electrolysis of unpolarized chloro-alkali will be mentioned, be the process of alkali metal chloride brines electrolysis, thereby wherein hydrogen evolution cathodic reaction is suppressed the reaction of oxygen consumption that is conducive on 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 technique electrolytic solution flows through suitable multi hole surface element or percolator under action of gravity: for example disclose such electrolyzer in WO/0157290.In such electrolyzer, typically there is the anodal compartment that is obtained 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 technique passes the multihole device that is inserted in cathodic compartment because of gravity flowage, 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 to 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 is because providing larger displacement contact and structure that can the mechanical support electrode to be affected.For improving electrochemical properties, also must (for example 0.1 arrive 0.5kg/cm with specified pressure 2) negative electrode is pushed into percolator, in order to allow electric continuity in the liquid electrolyte that helps the restriction circulation.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, consist of 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 be passed to enough pressure gas diffusion electrode and guarantee thus the electric continuity expected.Equivalent processes is for improvement of 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 gas diffusion electrode simultaneously, and described initial electrolysis groove negative electrode is the metal electrode that is used for liberation of hydrogen of being made by nickel or steel as known in the art.
Yet, aforesaid method also can be with and serve inconvenience, hindered the commercialization of this type electrolyzer: two element type current transmission system in fact related to expensive and thickness, installation difficulty and silk screen (particularly peripheral region) size control are difficult, be difficult to control distortion and elastic force, thereby certainly also exist in addition the increase contact interface not to be particularly conducive to ohmic voltage drop, for example the interface between silk screen and 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 for the diafiltration element of 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 for electrolyzer, this electrolyzer has gas diffusion electrode and percolator.
The present invention is comprised of the electrolyzer that has by the 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, the first interarea towards film contacts with the percolator that is passed by electrolyte stream, second interarea relative with the first interarea contacts with distributing switch, and this distributing switch comprises a plurality of elastic conductive thrusts that are applicable to gas diffusion electrode is pressed to percolator.As disclosed in WO/0157290, as percolator, expectation is suitable for any multi hole surface element that liquid stream passes 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 alloying differently, for example is selected from the classification of common obtainable product; Selection has the grade that is applicable to make 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 (tag) of arranging in pairs, and the interarea that makes the tinsel that two adjacent spring joints derive from from them is projection round about.Obtained by this way the more effective and uniform support of whole electrode surface.Such scheme is applicable to the almost best design of electrolysis cells of every kind of processing condition; Yet, use has advantages of the effective gas circulation of the permission (situation of depolarize chloro-alkali electrolysis for example according to the silk screen of prior art as the contact member under 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 one or more be used to the spring joint that electrically contacts being provided and one or morely being convenient to the opening that gas passes through successively.The for example parallel columns setting to distribute along whole electrode surface of conductive protrusions.
Be suitable for preferred 0.1 to 0.5kg/cm according to distributing switch of the present invention 2Pressure under directly realize effectively electrically contacting on the gas diffusion electrode surface, therefore need not the contact interface (in 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 gas diffusion electrode with being used for, 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 directly contacts with gas diffusion electrode the resistance that obtains lower than the almost nonelastic silk screen that makes prior art.In addition, those skilled in the art will readily understand, 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 the first embodiment according to distributing switch of the present invention.
-Fig. 4 has shown the 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) consists of its part, and the silk screen that elastic collector (210) is made by for example nickel consists of.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 consists of.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 consist of of such element; Anode substrate has catalyst coatings of separating out for chlorine commonly known in the art.Electric continuity between anode (302) and 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 consists of.Fig. 2 has shown foundation percolation type depolarize chloro-alkali of the present invention, and wherein the element identical with the electrolyzer of Fig. 1 adopts identical reference number mark.
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; Insert the selectable unit (230) that distributes mechanical compression force, for example thin net or porous chips or punched sheet between conductive protrusions (220) assembly and gas diffusion electrode (301).
Fig. 3 has shown an embodiment of a plurality of conductive protrusions that obtained by single tinsel, and the module composition of the elastomeric spring joint (221) that is arranged in parallel for how much by the foundation pectination in this situation: spring joint is arranged in pairs, makes every 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, the tetragon (222) that moulding obtains in this case, optional being welded direct on rigid current collector (201), each in them comprises the element with difference in functionality: for example, by suitable folding step, each watt acquisition has approximately the edge of 90 ° of bending angle (223), in order to 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) are conducive to supply and the circulation of gas, refers to especially in this case the oxygen that cathodic reaction needs.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 tinsel is punched sheet in this case, and extend on the whole main body of watt (222) that comprise spring joint (224) a plurality of holes (225 ').The gas that to strengthen is by this way supplied with, when spring joint (224) compressed and in the place of their projections when described contact this supply effectively, until the stroke end.Also obtain a small amount of the saving during making, the independent execution in the hole (225) shown in upper by watt (222) in Fig. 4 consists of.Watt structure further mechanics advantage also is provided: in unexpected high negative electrode counterpressure situation (for example because of the mistake of process regulation, perhaps because of the error of element operation or assembling), due to GDE whole watt lip-deep near, tension set does not occur 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 in Fig. 2, for having 0.16m 2The following element of use for laboratory experiment electrolyzer assembling of useful area: the titanium that possesses ruthenium and titanium oxide base catalyst coatings
Figure S2007800024095D00061
Anode (302), by Dupont/USA supply
Figure S2007800024095D00062
N982 ion-exchange membrane (500), nickel foam percolator, the gas diffusion electrode that is consisted of by the silver-colored net by the argentum-based catalyzer activation.
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 the temperature of 90 ℃ under, be the circulation sodium chloride brine of 210g/l to anode electrolytic cell compartment feed consistency.Cathode product is made of the caustic soda of 32 % by weight that are downward through percolator.Under these conditions, the stable process conditions on equipment after 10 days, is detected 2.00 to 2.05V bath voltage.
Embodiment 2
Utilize the test of the electrolyzer repetition embodiment 1 of prior art under simulated condition.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 the cathodic back-wall of being combined with commercial nickel screen.
Under the processing condition identical with embodiment 1, after 10 days, 2.10 to 2.15V bath voltage detected in stabilization.
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 (8)

1. electrolyzer, its type is the electrolyzer that comprises by the separated anodal compartment of ion-exchange membrane and cathodic compartment, described two compartments are equipped with one of at least gas diffusion electrode, this gas diffusion electrode has two interareas, the first interarea of described gas diffusion electrode towards described film and be suitable for the percolator that electrolyte stream passes contact under action of gravity, the second interarea of described gas diffusion electrode contacts with distributing switch, it is characterized in that, this distributing switch comprises a plurality of elastic conductive thrusts, described a plurality of elastic conductive thrust is suitable for described gas diffusion electrode is pressed to described percolator, and the described distributing switch that comprises described a plurality of conductive protrusions is to obtain by the cutting of single tinsel and moulding, and
Wherein said conductive protrusions is tetragonal independent watt, and described watt comprises a plurality of spring joints and at least one opening for gas circulation.
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. the electrolyzer of claim 1, the wherein said watt of parallel columns with skew is welded to rigid current collector.
4. claim 1 or 2 electrolyzer, wherein said tinsel has the thickness of 0.5 to 1.5 millimeter.
5. claim 1 or 2 electrolyzer, wherein said tinsel is punched sheet.
6. claim 1 or 2 electrolyzer, wherein said tinsel is made by nickel.
7. the electrolyzer of claim 6, the wherein said tinsel of being made by nickel has the coating that is suitable for reducing the contact resistance relevant to described thrust.
8. claim 1 or 2 electrolyzer, it comprises the add ons that is used for distributing mechanical compression force that is inserted between described distributing switch and 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)

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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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CN101370966B true CN101370966B (en) 2013-05-08

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