CN1292508C - Electrochemical system - Google Patents
Electrochemical system Download PDFInfo
- Publication number
- CN1292508C CN1292508C CNB2003801013314A CN200380101331A CN1292508C CN 1292508 C CN1292508 C CN 1292508C CN B2003801013314 A CNB2003801013314 A CN B2003801013314A CN 200380101331 A CN200380101331 A CN 200380101331A CN 1292508 C CN1292508 C CN 1292508C
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- Prior art keywords
- bipolar plates
- washer arrangement
- electrochemical
- compressor system
- perforation
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- Expired - Lifetime
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- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 4
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 4
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- 229910000851 Alloy steel Inorganic materials 0.000 description 1
- MYMOFIZGZYHOMD-UHFFFAOYSA-N Dioxygen Chemical compound O=O MYMOFIZGZYHOMD-UHFFFAOYSA-N 0.000 description 1
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 1
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- WYTGDNHDOZPMIW-RCBQFDQVSA-N alstonine Natural products C1=CC2=C3C=CC=CC3=NC2=C2N1C[C@H]1[C@H](C)OC=C(C(=O)OC)[C@H]1C2 WYTGDNHDOZPMIW-RCBQFDQVSA-N 0.000 description 1
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Images
Classifications
-
- 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
-
- 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
- C25B11/036—Bipolar 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
- 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
- C25B9/75—Assemblies comprising two or more cells of the filter-press type having bipolar electrodes
-
- 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
- H01M8/0204—Non-porous and characterised by the material
- H01M8/0206—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
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0247—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the form
- H01M8/0254—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the form corrugated or undulated
-
- 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
- H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
-
- 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
- H01M8/1007—Fuel cells with solid electrolytes with both reactants being gaseous or vaporised
-
- 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
- H01M8/24—Grouping of fuel cells, e.g. stacking of fuel cells
- H01M8/2465—Details of groupings of fuel cells
- H01M8/247—Arrangements for tightening a stack, for accommodation of a stack in a tank or for assembling different tanks
-
- 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
The invention deals with an electrochemical system for compressing gases and/or for producing gases by electrolysis, consisting of an electrochemical compressor stack (1) having layering of several electrochemical cells, which are separated from one another in each case by bipolar plates (3; 3'), wherein the bipolar plates have openings for media supply and media discharge (5a, 5b) for the electrochemical cells and the electrochemical cell stack can be placed under mechanical compressive strain in direction (6) of the layering. The bead arrangements (7; 7') are resilient and are provided at least in some regions to seal the openings (4, 5a, 5b) and/or an electrochemically active region (10) of the electrochemical cells.
Description
The present invention relates to a kind of electro-chemical systems, for example fuel cell system or electrochemical compressor system.
For example, electrochemical compressor system can be an electrolysis unit, and by applying voltage, it also under high pressure compresses these gases simultaneously except producing as water with by the water generates oxygen.
In addition, electrochemical compressor system for example electrochemical hydrogen compressor also is known, to wherein sending into gas molecule hydrogen, by applying voltage, with electrochemical means compression molecular hydrogen.This electrochemical compression is particularly useful for compressing small quantity of hydrogen, is quite expensive because adopt the mechanical system compression hydrogen this moment.
Known in electro-chemical systems, electrochemical cell is to be made of the stacked of several electrochemical cells, and described electrochemical cell is all isolated by bipolar plates in all cases mutually.Therefore, bipolar plates has following several effect:
-electrically contact with the electrode of each electrochemical cell and to adjacent battery (being connected in series of battery) transmission current,
-provide reactant to battery, for example water or gas, and for example remove the reacting gas of generation by suitable dispensing arrangement,
The heat that produces in-transmission electrochemical cell the power generation process, and
-make each medium tube or cooling water pipe with respect to other pipes and extraneous sealing.
Bipolar plates has and is used to cool off or the opening of medium supply and media discharge, be used for from bipolar plates to the electrochemical cell supply of reality and discharge medium (electrochemical cell of described reality is MEA (film electronic installation) for example, its have for example make by metal gasket, in all cases all towards the gas diffusion layers of bipolar plates).
Here often go wrong, especially about gas diffusion layers.So far, design for example being sealed between the bipolar plates or between bipolar plates and the electrochemical cell traditionally and in the groove of bipolar plates, elastomeric seal is set.By electrochemical cell being applied compression strain (for example by means of tension band), thereby taking place, sealing compresses, the result obtains the effect of opening sealing.
The problem that the gas diffusion layers that inserts exists at present is that this layer can be designed to fiber mat (use metallic fiber) or wire netting.Fiber mat conventional in the industry has for example theoretic throat of 1mm, but manufacturing tolerance is ± 100 μ m.The metallic fiber itself that makes up this pad only has a spot of elasticity.And, do not recommend by compressing the manufacturing tolerance that this fills up the compensation fibre pad yet, therefore because the gas permeation rate of this bed course is reduced greatly, and limit the work of electrochemical cell.But, on the other hand, must apply minimum pressure to whole gas diffusion layers by bipolar plates, make to have enough gas channels that passes gas diffusion layers.Thereby can be summarized as follows,, always have the situation of not exclusively sealing or the non-best effort of electrochemical cell for present elastomeric seal.And, especially for the electrochemical cell that uses molecular hydrogen work, the H through the elastomeric seal diffusion can take place
2Seepage loss.
Therefore, as first aspect, the objective of the invention is with the positiver sealing of alap cost realization to the opening in the electrochemical cell.
Above-mentioned purpose is realized by electrochemical compressor system of the present invention.
By being provided for the elastic washer device of sealed open at least in some zone, obtain sealing reliably along the resilient path of the length of washer arrangement.In fact, opening should be understood that any zone to be sealed in this application.It can be for example to be used for reacting fluid (H for example
2Or water) or the passway of cooling agent.But it also can be for example electro-chemical activity zone that wherein for example is provided with gas diffusion layers or is provided with screw hole.This elastic washer device always allows to compensate for example manufacturing tolerance of gas diffusion layers in the big margin of tolerance, and best sealing effectiveness still is provided.
It is that 1 μ m-400 μ m thin layer carries out little sealing (microsealing) that a very favorable embodiment imagination of the present invention is designed to used thickness with washer arrangement.Advantageously, this thin layer by elastomer for example silicones, fluorubber or EPDM (ethylene/propene-diene terpolymer) make, preferably (sealing gasket (in place) on the spot solidifies by silk-screen printing technique, bat printing technology, spraying or CIPG; It is the elastomer that is introduced into sealing station and solidifies in this position with liquid form) apply.These methods are guaranteed for example to be reduced to an extremely low level by the diffusion that seals hydrogen, but this is because the height of permeability material is adjusted to minimum value.Therefore do not attempt to regain extra geometric height, but only attempt the roughness compensation is carried out in little sealing.
Another advantageous embodiment imagination washer arrangement of the present invention comprises full packing ring or half packing ring.Thereby these two kinds of forms also can be provided in washer arrangement, because according to the horizontal route of washer arrangement, other elasticity prove useful, for example except the straight line path for washer arrangement, when radius hour, different gasket geometries is useful.
A favourable improvement of washer arrangement is to imagine at least in some zone washer arrangement to be designed to half packing ring, and it is provided with around the electro-chemical activity zone and is regional around electro-chemical activity zone opening at some.Fix this half packing ring, make it, thereby guarantee to press, packing ring is increased the contact pressure of the sealing surface (or therebetween film) of adjacent bipolar plates by in increasing towards the high-pressure side opening.Since externally stablized the electrochemical compression unit by the end plate of using tension band etc. to be fixed together, therefore only can be on limited degree, each plate that can obtain piling up.Whole device does not have " elastic dilatation ", and only increases contact force at seal area, to such an extent as to even the self-stable function of existence sealing or whole device.Thereby with half gasket design (interior pressure can be clung to greater than 200 for the system pressure by increasing the electro-chemical activity zone, be preferably greater than 700 crust, be preferably greater than 1000 crust especially, the highest 5000 crust), the surface pressing that points to the direction of electrochemical compression unit increases, to such an extent as to got rid of the compactness problem and provide accurate " self-stabilization " system at sealing.
Another advantageous embodiment imagination washer arrangement is formed from steel.The advantage of steel is to use conventional instrument very at low cost it to be processed, and for example the method to the thin elastomer layer of steel coating all is to pass through severe test.According to the present invention, the better elastic performance of steel helps successfully designing the elastic packing district of length of the present invention.Thereby especially washer arrangement can be fixed on the bipolar plates.Thereby, at first can be with the moulded parts (can be provided with corrosion-resistant or conductive coating) of whole bipolar plate design Cheng Gang in some zone.But, also bipolar plate design can be become to have the composite component of two steel plates of plastic plate therebetween.But, under the various situations of the good machinability that can use steel, make washer arrangement (for example stream field carries out mold pressing, i.e. " fluid field ") in the production stage that can both under any circumstance carry out.The result produces low-down cost, and the elastomeric seal that extra assembly for example additionally inserts does not provide extra source of error.
But,, also can provide by other metals washer arrangement of making of steel, nickel, titanium or aluminium and alloy thereof for example according to the present invention.This selection of preferable alloy also depends on for example required electrical property or required corrosion-resistant degree.
Thereby can adjust the compression property of packing ring, for example make it to adapt to gas diffusion layers.But it needn't be only applicable to gas diffusion layers, the assembly that common packing ring sideline is very suitable for having low elasticity.Can design the flanging sealing neatly, thereby can be used well, and bring high renovation cost can for the manufacturer of electrochemical compressor system.
Another advantageous embodiment imagination washer arrangement has stop, and it will be restricted to minimum thickness to the compression of gas diffusion layers.It is the incompressible part or the parts of washer arrangement, and its elasticity is far below the elasticity of actual bead.This has just guaranteed that the deformation extent in gasket areas is limited, to such an extent as to can not there be the pressing fully to packing ring.
Another advantageous embodiment imagination is with on the assembly that washer arrangement is arranged on bipolar plates is separated.Be particularly advantageous in when bipolar plates be when constituting by the material that is not suitable for washer arrangement.Then, independent assembly is installed on the bipolar plates, or by bonding, pour (clicking-in), welding (welding-in), soldering (soldering-in) or casting and combine, thereby between independent assembly and bipolar plates, realize being tightly connected fully.
At last, another advantageous embodiment imagination is by elastomeric roller design washer arrangement.Can apply this packing ring by silk-screen printing technique or bat printing.This packing ring can be used for little sealing and macroscopic view sealing (macrosealing).This cylinder also supposes to have the function of the road coupling on the gas diffusion layers.
Another favourable improvement imagination is designed to electrolysis unit with electrochemical compressor system.Here, the water that will introduce electrochemical cell one side with electrochemical method resolves into hydrogen molecule and oxygen molecule.Film of being made by Nafion or similar proton conduction system are used for this purpose, but also can use the separator that for example comprises the PTFE foamed plastics that soaks with potassium hydroxide.And the porous ceramic structure that soaks with potassium hydroxide is possible separator, for example based on structure or the hydroxide transmission structure of Nextel.Contact force (surface pressing of the sealing on the principal direction of electrochemical cell) can be 0.1-200N/mm
2, be preferably greater than 10N/mm
2, be preferably greater than 50N/mm especially
2
Another favourable improvement imagination electrochemical compressor system is a hydrogen compressor, and its molecular hydrogen that will introduce on first of proton conduction electrochemical membrane is oxidized to H
+, and on second, again it is reduced to molecular hydrogen, wherein owing to seal and space layout, molecular hydrogen there is bigger at the pressure that the pressure ratio that is subjected on second is subjected on first.Here, working temperature should be 0-100 ℃, and 0-200 ℃ or 0-550 ℃ also is feasible.Here, can use the hydroxide transmission structure or even known protonically conductive polymer film (for example making) by Nafion be used as film.
Certainly, also can correspondingly compress other gas, be used for selecting suitably ion conductor, for example have the oxygen of hydroxide transmission structure.
Generally, should remember that described electrochemical compressor system should stand very big pressure as much as possible, the pressure that this pressure adopts in other electrochemical machinery devices.Do not having under the situation of leakage loss, the leading air pressure in the electro-chemical activity zone should be at least 100 crust, is preferably greater than 200 crust, is preferably greater than 500 crust especially.
Second aspect of the present invention relates to the purpose that makes the opening realization positiver sealing in the electrochemical cell with alap cost, wherein should guarantee to supply safely the medium that is used to cool off and be used for electrochemical cell work (O particularly, from the opening to the cooling chamber or towards the electro-chemical activity zone of electrochemical cell
2Or air or H
2).This respect can be used for any electro-chemical systems, for example fuel cell or above-mentioned electrochemical compressor system.
The realization of purpose of the present invention is in the around openings of at least one bipolar plates the elastic washer device to be set, and wherein is used for the perforation pattern of fluid transfer or gas medium at least one side in washer arrangement.An electrochemical compressor system (perhaps being used for fuel cell system) of being made up of the electrochemical cell (perhaps fuel battery) with stacked several electrochemical cells (or fuel cell) is shown here, described battery is all separated by bipolar plates in all cases, wherein bipolar plates has the cooling that is used for electrochemical cell (fuel cell) or is used for the opening of supply of its medium and media discharge, and can under the mechanical compress strain of stacked direction, electrochemical cell (or fuel battery) be set, wherein the elastic washer device wherein is provided for the perforation of fluid transfer or gas medium around the opening setting of bipolar plates at least one side of washer arrangement.
At first, when applying mechanical pressure on the stacked direction of electrochemical cell, at first realize the sealing of opening usually by washer arrangement, this is particularly advantageous, and described sealing is cheaply and good tolerance compensating is provided.In addition, the perforation on the washer arrangement side helps specifically supplying or discharging cooling agent and supply reliably and discharge medium in corresponding coolant cavity.No longer need to block packing ring fully so that accurate stacked direction (overlapping) supply or discharging cooling agent or operation medium with the direction of interface pipeline perpendicular to electrochemical cell.Therefore, can provide corresponding perforation in the process of making these bipolar plates, described perforation caused the medium supply in the final electrochemical compressor system afterwards.Therefore, advantageously, these perforation can be made on a large scale, easily, the flow resistance of washer arrangement and rigidity etc. can be accurately preset by changing these perforation.
Especially can save local bipolar plates or its parts made, owing at first the hole being set on metallic plate, then carry out the mechanical-moulded to make washer arrangement of orifice plate, the hole of introducing before making becomes the perforation of at least one side that is positioned at washer arrangement.Certainly, also the profile of at first mold pressing bipolar plates for example uses laser processing, punching press (punchsupply) to wait and introduce perforation then.
Therefore, can be summarized as, value of the present invention is to simplify the medium supply to the active region of bipolar plates." tunnel effect " of sealing is optional, because the medium supply of this moment is undertaken by sealing system itself.This first has saved the space, and second helps improving the capacity and the weight capacity of electrochemical cell.Particularly, the present invention can be used for the bipolar metal plates of PEM electrochemical cell, and in most of the cases described metallic plate is to be made of two embossed metal sheets that mutual plane connects.WATER AS FLOW MEDIUM is that cooling water and gas must be sealed effectively mutually in some cases.If the sealing of bipolar metal plates is designed to gasket construction, then in most of the cases the packing ring position that should flow into the active region at medium is seriously flattened.The supporter that does not have film in these positions, this can cause gas leakage (" connecting (cross-over) ") or cause film to cave in to service duct.But, if introduce perforation in the side of packing ring and allow medium for example hydrogen, air, distilled water cross-current enter the flow field area of bipolar plates through packing ring, then packing ring can be resisted against on the not intercepted film.Obtain the sealing fully of MEDIA FLOW thus.In order to change the elastic characteristic of packing ring indistinctively, more advantageously the hole is designed to circle or ellipse.By being applicable to that MEDIA FLOW has guaranteed sealing between the fluid that occurs in the electrochemical cell flows through the design of second metallic plate of the bead construction in zone.Thereby packing ring can design and helps packing ring or half packing ring.And MEDIA FLOW is through having the packing ring of continuous pipeline.This is especially favourable for guided.Thereby guided is more easy between positive plate and minus plate.
The cross section that the perforation of another favourable improvement imagination side plane can have circle, ellipse or the angle is arranged.The mobile performance of fluid of these perforation of being directed flowing through at first is subjected to the influence of suitable the number of holes of this shape and each side plane.And, for the stress on the stacked direction of electrochemical cell, can also control the rigidity of washer arrangement, the common influence of shape because corresponding how much moments of inertia also are subjected to boring a hole.
A particularly advantageous improvement imagination is connected to a perforation with a pipeline, and wherein pipeline is connected to bead interior and at least towards the bead outer surface closure.This has just guaranteed that perforation is not directly to be directed to its outside from bead interior, but can carry out specific transmission by the pipeline in the hydrogen groove of for example bipolar plates; Therefore can prevent from oxygen is introduced the negative electrode of electrochemical cell.With regard to manufacturing technology, particularly advantageous is these pipelines of co-molded in mold pressing bipolar plates (for example when it is made of metal), perhaps, and in the back or formerly to fix each pipeline all be feasible certainly.
Another improves the imagination perforation towards the electro-chemical activity zone of electrochemical cell opening.This especially is used to introduce for example hydrogen of medium.Certainly, in single bipolar plates, also can there be the different variants that adjoin each other simultaneously, promptly be connected to the perforation of pipeline and do not have the perforation of pipeline.
One is made of two (metal) plates in industrial very promising embodiment imagination bipolar plates, and between two boards, it has to be positioned at and is used for cooling agent and/or dielectric gas such as H between the two
2The chamber of passing through.Therefore, the inside of this bipolar plates can also be divided into several portions, for example is divided into the part that is used for conduct coolant on the one hand and is used for distribution media gas on the other hand.This division can be provided by the join domain of two boards, and it is designed to for example weld or soldering.
Another favourable improvement imagination washer arrangement comprises " full packing ring " or " half packing ring ".For full packing ring, can select to establish on one or both sides perforation.Needing full packing ring still is that half packing ring especially depends on required rigidity or also depends on the physical dimension of opening.
Washer arrangement is particularly suitable for by the metal bipolar plates that constitutes of steel, nickel, titanium or aluminium and alloy thereof for example.Washer arrangement can be the part of topography embossed in the bipolar plates.But, also washer arrangement can be arranged on the assembly, described assembly at first separates with bipolar plates, then be arranged on especially on the bipolar plates of making by metal, plastics, graphite etc., perhaps by bonding, pour (clicking-in), welding (welding-in), soldering (soldering-in) or casting and be connected on the bipolar plates.
Another favourable improvement imagination applies washer arrangement and is used for little sealing.This has guaranteed that for example by means of the elastomer layer that applies in the outside of washer arrangement by silk-screen printing technique, realization prevents little sealing that medium passes through.This elastomer coating also has extra effect, promptly settling on this layer under the situation of polymer film, provide " floating type " or " slidingtype " fixing, this has guaranteed on the one hand even for about 10% change in size, the film of this electrochemical cell is still fixing, and on the other hand because rigidity fixing too, the crack does not appear in film.
Another favourable improvement imagination is arranged on the electro-chemical activity zone of electrochemical cell in the airtight substantially chamber, and this chamber is subjected to the lateral limitation substantially in the form of a ring of washer arrangement.This means that washer arrangement not only can be used for sealing the opening of bipolar plates, and inside that can " integral sealing " electrochemical cell.
A particularly advantageous improvement imagination, in perforation and the not perforated side regions, along the stress of the stacked direction of electrochemical cell, washer arrangement has essentially identical rigidity.Can adjust to identical rigidity by different modes.For example can be by means of adjusting along the angle of the flank (flank angle) (for example steeper angle of the flank in the side regions of perforation) of the path change of washer arrangement or by suitable distribution of material (i.e. the bigger wall thickness in next-door neighbour peripheral region of for example boring a hole).For example can use ultimate tensile strength Rm to be 300-1,100N/mm
2, preferred 600-900N/mm
2Steel.The modulus of elasticity of these steel is 150,000-210,000N/mm
2
Set forth the present invention below in conjunction with accompanying drawing.
Fig. 1 a-1c illustrates the structural type of electrochemical cell,
Fig. 2 aa, 2ab and 2b illustrate the embodiment of washer arrangement of the present invention,
Fig. 2 c illustrates the plane graph of bipolar plates of the present invention,
Fig. 3 a-3d illustrates several washer arrangement that has stop,
Fig. 4 illustrates digging of industrial bipolar plates and cuts figure (cutout),
Fig. 5 a and 5b illustrate the schematic diagram of the washer arrangement with perforation,
Fig. 6 a-6c illustrates the schematic diagram that has the perforation and be connected with the washer arrangement of pipeline,
Fig. 7 a-7c illustrates the dissimilar of washer arrangement design of the present invention,
Fig. 1 a illustrates the structure of electrochemical cell, shown in Fig. 1 b.A plurality of electrochemical cells form the zone (shown in Fig. 1 c) that is arranged in the electrochemical cell 1 between the end plate with overlapped way.
The access portal 5a that is used for the medium supply is positioned at sealing area with the access portal 5b that is used for media discharge, by packing ring 11 it is sealed with respect to the access portal 4 (it has independent seal washer, and this packing ring is provided with according to the present invention equally) that other access portal for example are used to cool off.By on stacked direction 6, electrochemical cell 1 being exerted pressure, on all packing rings, all realized sealing effectiveness (seeing Fig. 1 c).This realizes by for example unshowned here tension band.The advantage of packing ring 11 is that it has the big elastic compression zone that shows sufficient sealing effectiveness.This is especially favourable when gas diffusion layers 9 is installed, and described gas diffusion layers 9 is made by for example graphite or metallic fiber pad (titanium, stainless steel or nickel), and the gas diffusion layers 9 of industrial production has big manufacturing tolerance.Because the elastic range of packing ring 11 is wide, it is feasible therefore packing ring being adjusted to the physical dimension that is fit to gas diffusion layers.This has guaranteed to provide on the one hand lateral seal, and it is uniform and enough big that enough gas dispersion and contact pressures on the stacked direction 6 are provided in the gaseous diffusion layer plane on the other hand, thereby makes the even gas coming through anemostat of air-flow.In order to improve little sealing, provide elastomeric coating in the outside of packing ring 11, this coating applies by for example silk-screen printing technique.
In order to limit the extruding to gas diffusion layers, the design gasket construction has stop.This stop can be designed to folding, ripple stop or even trapezoidal stop, with in the back at this stop is described in the description of Fig. 3 a-3d in further detail.All stops all have and can will be restricted to the effect of a minimum dimension to the compression of packing ring.
In this case, bipolar plate design is become the metal pattern product.Referring to the described content of advantage at the production convenience and the steel of binding washer device.
If bipolar plates is to form by for example being not suitable for making the metal forming with must be flexible suitable gasket geometries, then gasket areas can be designed to make by different suitable material (for example steel).Then by joint technology, for example welding, soldering, bonding, rivet, pour (clicking-in), independent gasket assembly is connected to bipolar plates.If bipolar plates is to be made by the material except that metal, for example make by graphite composite, plastics or graphite, then gasket areas can be designed to the framework of making by suitable material.By joint technology, for example fuse, cast, welding, soldering, bonding, rivet, pour, the base material that will comprise the bipolar plates in flow field is connected to the washer sealing framework that comprises packing ring with airtight or the close mode of liquid.
Fig. 2 aa and 2ab illustrate the embodiment according to washer arrangement of the present invention.Fig. 2 aa illustrates the cross section that passes the washer arrangement 7 that is designed to half packing ring.Substantially in the form of a ring packing ring 11 sealing gas diffusion layers 9, this point is expressed in the design of Fig. 1 a.In Fig. 2 aa, packing ring is designed to so-called half packing ring, promptly for example similar quadrant.Because the interior zone of electrochemical cell must be sealed by sealing gasket, and, therefore need another kind of the design, promptly be designed to full packing ring or half packing ring in medium pipeline zone existence intersection (seeing Fig. 2 c).A full packing ring can change two and half packing rings into, and they itself all have sealing function in all cases.And, use full packing ring or half packing ring to provide and in big frame structure, change flexible possibility.
Fig. 2 aa illustrates the washer arrangement 7 that is in the not subjected to pressure state.When electrochemical cell is applied the mechanical compress strain, on direction 6, push, to such an extent as to washer arrangement 7 or packing ring 11 form the air-tightness lateral seal of confined chamber with respect to gas diffusion layers.
Fig. 2 ab washer arrangement 11 is shown another dig and cut figure.It is designed to half packing ring.This half packing ring or the washer arrangement with half packing ring form are connected to bipolar plates 3 by welded side seam 27.Film 2 be arranged on half packing ring above, this half packing ring is designed to serpentine basically.Therefore, electro-chemical activity zone tunicle 2, half packing ring 11 and bipolar plates seal with air tight manner, to such an extent as to press P in this forms
InternalBy the metallic fiber pad, be to be positioned in the electro-chemical activity zone here by the gas diffusion layers that the titanium fiber mat is made.At least the set-up mode in some regional half washer arrangement is: because the increase of the pressure in electro-chemical activity zone is pressed P in causing
InternalIncrease, thereby upper side that will " S " upwards promotes (also seeing broad arrow), and the therefore surface pressing increase in the upper side of " S ".Because during the integral body on the electrochemical cell direction is extended, whole electrochemical cell is limited by tension bands to a minimum dimension, therefore exist the interior surface pressing of this side regions to increase, and thereby produce better sealing, standard " self-stabilization system " that Here it is.
Fig. 2 b illustrates another washer arrangement, i.e. washer arrangement 7 '.This device is designed to full packing ring (approximately having semi-circular cross-section) with the unique different packing rings herein that are of Fig. 2 a shown device.The present invention also has many other embodiments.Therefore, for example can demonstrate with here shown in other different gasket geometries, also can be many packing rings.And washer sealing of the present invention can be used for all sealing gaskets in the electrochemical cell zone of pressurized.Not only can center on gas diffusion layers sealed electrochemical active region 10, and can sealing gas or any passage of liquid medium etc.For the sealing of the assembling guider (screw hole) that centers on electrochemical cell, can utilize the elasticity of washer arrangement, thus the installation process of revertive control battery pack (settling process), and compensate possible tolerance.
Fig. 2 c illustrates the plane graph of another embodiment of bipolar plates 3 ' of the present invention.In this plane graph, represent washer arrangement with thick line.Thereby washer arrangement is used to seal several access portal.
Fig. 3 a-3d illustrates the various washer arrangement that have stop.This stop is used to limit the deformation of packing ring, makes packing ring not to be compressed into and surpasses certain size.
Therefore, Fig. 3 a illustrates has full packing ring 11 " the single-layer pad coil apparatus, on direction 15, arrive the deformation limit of these full packing rings by ripple stop 29.Fig. 3 b illustrates double-layer bead ar-rangement, and the deformation of its complete at the middle and upper levels packing ring is limited by the folded metal pad (seeing Reference numeral 34) that is positioned under it.Fig. 3 c and 3d illustrate wherein at least two full packing rings be in relative position and provide folding mat (seeing Fig. 3 c) or ripple pad (seeing Fig. 3 d) with the washer arrangement of restriction deformation.
Fig. 4 illustrates the detailed structure that digging of bipolar plates 3 cut figure, and the front has used Fig. 1 a on principle it to be illustrated.This bipolar plates can be used for any electro-chemical systems in principle, promptly for example is used for above-mentioned electrochemical compressor system or fuel cell system.
Opening 5a or 5b are centered on by full packing ring, are used for to electro-chemical activity zone supplying media, for example H
2Or water.Washer arrangement 7 around opening 5 has hole type perforation 8, and it allows on the direction of arrow 18 through perforation 8 supplying medias.
Opening 4 is used for the gap supply cooling fluid body between metallic plate 3a and 3b.Opening 4 is centered on by washer arrangement 7 '.The pipeline 28 that is connected to unshowned perforation 8 ' (sees that Fig. 6 a) enters the inside of bipolar plates 3 from washer arrangement.
Fig. 5 a illustrates and two cuts figure in digging of the upper plate 3a that cuts open pole plate 3.In the washer arrangement 7 that centers on opening 5a or 5b shown in the cross-sectional view.As shown in Figure 4, this section is corresponding to hatching A-A.In cross-sectional view, washer arrangement 7 illustrates full packing ring, promptly is connected to the rising side 7b of plane domain (around opening) and the descending profile 7a that is connected to another level board after a level board.Side 7b and 7a have circular hole 8, and gas is H for example
2Supply represent with corresponding arrow (they are corresponding to the direction of arrow among Fig. 4 18).Certainly, also can provide oval or angled perforate, half packing ring that has only the descending profile that begins from horizontal zone perhaps only is provided.Opening 8 is towards the electro-chemical activity of electrochemical cell 2 zone 10 or bipolar plates 3 openings, to such an extent as to medium fluid for example air, H
2Perhaps water can pass through thus.In other designs, have only a side for example side 7a to comprise perforation also be feasible certainly.
Fig. 5 b illustrates the bipolar plates 3 in electrochemical cell or fuel cell or the electrochemical compressor system.Show around digging of opening 5 and cut figure as " interface " pipeline.The electrochemical cell 2 that is connected with bipolar plates (not shown in some cases) in turn all is set at the above and below of bipolar plates 3 in all cases, for explanation better, saves the narration to independent gas diffusion layers.The gas that flows into from the interface pipeline is basically along the direction 19 interface pipeline of flowing through.Main flow direction in the pipeline of interface is represented with arrow 19, carry out along the direction of arrow 20 between the top and electrochemical cell 2 that further is dispersed in bipolar plates 3 of the gas in the electro-chemical activity zone 25, and since the suitable cavity shape of bipolar plates can further disperse by cavity 4.Molecular hydrogen can also be in the corresponding way promptly flows through on the zone 21 in another planar side of bipolar plates 3.
Fig. 5 b shows again and how by engaging zones 26 cavity 14 and the cavity 13 that fills cooling liquid to be separated.
Fig. 6 a illustrates digging of washer arrangement 7 ' and cuts figure, and it shows the peripheral region (according to section B-B) of opening 4.
Washer arrangement 7 ' has full packing ring.This full packing ring has perforation 8 ' on the 7a ' of its side, in the outside of washer arrangement, pipeline 28 is connected to this perforation.Pipeline 28 is guaranteed to be provided with connection in bead interior, and therefore the gas that flows along direction 22 can not flow to bead outer surface 35.
Fig. 6 b illustrates the section that passes a part of electrochemical cell once more, specifically in the zone around opening 4 (opening belongs to the interface pipeline that for example is used for cooling agent, and at this, cooling agent is a distilled water).These water flow along direction 23 usually, and a part of current are shunted on direction 24 and entered the cavity 13 that holds cooling liquid.Therefore can be clear that in Fig. 6 that by being connected to the pipeline 28 of perforation 8 ', cooling liquid flows in the cavity 13 like clockwork, between plate 3a and the electrochemical cell above it 2 and O is housed
2 Zone 25 liquid contamination that is not cooled.
Fig. 6 c illustrates the detailed plane graph around the zone of opening 4 once more.Corresponding small-sized the digging that shows the upper plate 3a of bipolar plates 3 cut figure.Can be clear that especially, provide washer arrangement 7 ' around opening 4, the pipeline 28 of direct coolant body inflow cavity 13 (entering paper plane) is connected to the side 7a ' of washer arrangement 7 '.
Provide washer arrangement of the present invention especially to be used for and to save into the bipolar plates that local produced in series has required tightness with high quality standards.The structure of the bipolar plates with whole washer arrangement especially is provided.Can be by the whole washer arrangement of making of metal sheet, for example by mold pressing (for example in the mold pressing pipeline configuration), the result makes production cost very low.Especially do not need to adopt extra black box, it is expensive that extra assembly is set.
Fig. 7 a-7c illustrates the different embodiment of washer arrangement.All these washer arrangement all can be used for above-mentioned washer arrangement, to limit electro-chemical activity zone or opening and hole.For explanation better, represent washer arrangement with new Reference numeral 30-33 below.
Fig. 7 a illustrates different may the changing of washer arrangement at first by way of example with the 3D position.This relates to the particular path (seeing Fig. 2 b or Fig. 5 a (washer arrangement 7) or the 6a (washer arrangement 7 ') that for example have washer arrangement 7 ') of full packing ring.Corresponding path also is applicable to full packing ring.About other details, with reference to foregoing.
It is wide that washer arrangement 31 illustrates variable bar, and it can be provided to optional frequency f equally." bar is wide " is interpreted as outer wide corresponding to the last plat part of the bar that defines among Fig. 7 c wide " stb ".For washer arrangement 31, bar is wide between stb1 and stb2 alternately (stb1 can be 0.1-5mm, and stb2 can be 0.2-10mm).
At last, it can also be seen that washer arrangement 30 illustrates the packing ring with variable edge width.For example change border width successively with predetermined frequency f.In order accurately to define border width, referring to Fig. 7 c, there, " scb " has been defined as the size (outer surface in bipolar plates records) of border width, for the washer arrangement 30 that illustrates here, border width replaces (scb1 can be 0.3-5mm, and scb2 can be 0.2-3mm) between scb1 and scb2.
Claims (43)
1. electrochemical compressor system of coming Compressed Gas by electrolysis and/or producing gas, it is made up of the stacked electrochemical compression unit (1) with some electrochemical cells, and described electrochemical cell is by bipolar plates (3; 3 ') it is isolated mutually, wherein bipolar plates has the medium supply that is used for electrochemical cell and the opening (5a of media discharge, 5b), and electrochemical cell wherein provides flexible washer arrangement (7 at least along settling under the mechanical compress strain of stacked direction (6) in some zone; 7 '), with sealed open (4,5a, 5b) and/or the electro-chemical activity zone (10) of electrochemical cell, and described washer arrangement is made of metal, wherein bipolar plates (3; 3 ') being designed to bulk metal moulded parts and/or described washer arrangement is the plate (3a that belongs to bipolar plates; Part 3b).
2. the described electrochemical compressor system of claim 1 is characterized in that described electrochemical cell has the gas diffusion layers of being made by conducting structure (9) in the face of on the face of bipolar plates.
3. the described electrochemical compressor system of claim 2 is characterized in that described conducting structure is a metallic fiber.
4. the described electrochemical compressor system of claim 1 is characterized in that described washer arrangement (7; 7 ') coated, thus little sealing medium.
5. the described electrochemical compressor system of claim 4 is characterized in that described coating use elastomer carries out.
6. claim 4 or 5 described electrochemical compressor system is characterized in that solidifying on the spot by silk-screen printing technique, bat printing, spraying or sealing gasket and coat.
7. the described electrochemical compressor system of claim 1 is characterized in that described washer arrangement (7; 7 ') comprise full packing ring or half packing ring.
8. the described electrochemical compressor system of claim 1 is characterized in that described washer arrangement (7; 7 ') make by steel, nickel, titanium or aluminium and alloy thereof.
9. the described electrochemical compressor system of claim 1 is characterized in that described washer arrangement has the stop that the compression of gas diffusion layers is restricted to minimum thickness.
10. the described electrochemical compressor system of claim 1 is characterized in that described washer arrangement (7; 7 ') be connected to bipolar plates (3; 3 ').
11. the described electrochemical compressor system of claim 1, it is characterized in that on described washer arrangement is arranged on bipolar plates is separated the assembly, described component placement is by graphite, plastics, above the metal bipolar plates, or by bonding, pour, welding, soldering or casting be connected with bipolar plates.
12. the described electrochemical compressor system of claim 9 is characterized in that described bipolar plates (3; 3 ') be designed to have the composite component of two metallic plates of plastic plate therebetween.
13. the described electrochemical compressor system of claim 1 is characterized in that the electro-chemical activity zone of electrochemical cell is arranged in the airtight chamber, this chamber is by washer arrangement lateral limitation ringwise.
14. the described electrochemical compressor system of claim 13 is characterized in that at least in some zone described washer arrangement is designed to half packing ring towards electro-chemical activity zone (10) opening.
15. the described electrochemical compressor system of claim 1 is characterized in that described washer arrangement is designed to elastomeric roller, by silk screen printing or bat printing or mold pressing it is applied as cylinder.
16. the described electrochemical compressor system of claim 1 is characterized in that the water decomposition that electrolysis unit will be introduced a side of electrochemical cell with electrochemical means is molecular hydrogen and oxygen.
17. the described electrochemical compressor system of claim 1, it is characterized in that the molecular hydrogen that hydrogen compressor will be incorporated on first of the proton conduction electrochemical cell is oxidized to H+, and on second, once more H+ is reduced to molecular hydrogen, wherein owing to seal and space layout, molecular hydrogen there is big at the pressure that the pressure ratio that is subjected on second is subjected on first.
18. the described electrochemical compressor system of claim 1 is characterized in that the air pressure in the sealed electrochemical active region, making is not having under the situation of leakage loss, and the leading air pressure in confined chamber is greater than 100 crust.
19. the described electrochemical compressor system of claim 1 is characterized in that the air pressure in the sealed electrochemical active region, making is not having under the situation of leakage loss, and the leading air pressure in confined chamber is greater than 200 crust.
20. the described electrochemical compressor system of claim 1 is characterized in that elastic washer device (7; 7 ') around bipolar plates opening (4; 5) and/or the electro-chemical activity zone provide, the perforation (8,8 ') that wherein will be used for conductive liquid or gas medium is arranged at least one side (7a, 7a ') of washer arrangement.
21. the described electrochemical compressor system of claim 19 is characterized in that described perforation (8,8 ') is circular, ellipse or dihedral.
22. claim 20 or 21 described electrochemical compressor system is characterized in that pipeline (28) is connected to perforation (8 '), wherein this pipeline are connected to bead interior (10 ') and at least towards the outer surface closure of packing ring.
23. claim 20 or 21 described electrochemical compressor system is characterized in that described perforation (8) is towards the electro-chemical activity zone of battery opening.
24. the described electrochemical compressor system of claim 20 is characterized in that (3a 3b) constitutes described bipolar plates (3), has the cavity (13 that is used for cooling agent and/or transmission medium fluid between described two plates by two plates; 14).
25. the described electrochemical compressor system of claim 7 is characterized in that full packing ring is in a side (7a) or two side (7a; Comprise perforation (8 7b); 8 ').
26. the described electrochemical compressor system of claim 1 is characterized in that for perforation being arranged and not having the stress of (6) on the inner stacks direction of perforated side zone, described washer arrangement (7; 7 ') has identical rigidity.
27. be used for the bipolar plates of the described electrochemical compressor system of claim 1, wherein said bipolar plates has elastic washer device (7,7 '), described washer arrangement is made of metal and described bipolar plates (3; 3 ') being designed to bulk metal moulded parts and/or described washer arrangement is the plate (3a that belongs to bipolar plates; Part 3b).
28. fuel cell system, it constitutes by having the stacked fuel battery (1) of some fuel cells (2), described fuel cell is isolated it mutually by bipolar plates (3), wherein bipolar plates has the opening (4) of the cooling that is used for fuel cell or is used for the opening (5a of medium supply and media discharge, 5b), and fuel battery wherein centers on the opening (4 of bipolar plates along settling under the mechanical compress strain of stacked direction (6); 5) provide elastic washer device (7; 7 '), the perforation (8,8 ') that wherein is used for fluid transfer or gas medium is set at least one side (7a, 7a ') of washer arrangement, and described washer arrangement is made of metal, and wherein bipolar plates (3; 3 ') being designed to bulk metal moulded parts and/or described washer arrangement is the plate (3a that belongs to bipolar plates; Part 3b).
29. the described fuel cell system of claim 28 is characterized in that described perforation (8,8 ') is circular, ellipse or dihedral.
30. claim 28 or 29 described fuel cell systems is characterized in that pipeline (28) is connected to perforation (8 '), wherein this pipeline are connected to bead interior (10 ') and at least towards the outer surface closure of packing ring.
31. claim 28 or 29 described fuel cell systems is characterized in that described perforation (8) is towards the electro-chemical activity zone (10) of fuel cell opening.
32. the described fuel cell system of claim 28 is characterized in that (3a 3b) constitutes described bipolar plates (3), has the cavity (13 that is used for cooling agent and/or transmission medium gas between described two plates by two plates; 14).
33. the described fuel cell system of claim 28 is characterized in that described washer arrangement (7; 7 ') comprise full packing ring or half packing ring.
34. the described fuel cell system of claim 33 is characterized in that full packing ring is in a side (7a) or two side (7a; Comprise perforation (8) 7b).
35. the described fuel cell system of claim 28 is characterized in that described washer arrangement (7; 7 ') constitute by steel, nickel, titanium or aluminium.
36. the described fuel cell system of claim 28 is characterized in that described washer arrangement (7; 7 ') be the part of the plate (3a) that belongs to bipolar plates.
37. the described fuel cell system of claim 28, it is characterized in that on described washer arrangement is arranged on bipolar plates is separated the assembly, described component placement is by graphite, plastics, above the metal bipolar plates, or by bonding, pour, welding, soldering or casting be connected with bipolar plates.
38. the described fuel cell system of claim 28 is characterized in that described washer arrangement (7; 7 ') coated, thus little sealing medium.
39. the described fuel cell system of claim 28 is characterized in that the electro-chemical activity zone of fuel cell is arranged in the airtight chamber, this chamber is by washer arrangement lateral limitation ringwise.
40. the described fuel cell system of claim 28 is characterized in that for perforation being arranged and not having the stress of (6) on the inner stacks direction of perforated side zone, washer arrangement (7; 7 ') has identical rigidity.
41. be used for the bipolar plates of the described fuel cell system of claim 28, wherein said bipolar plates has elastic washer device (7,7 '), described washer arrangement is made of metal and described bipolar plates (3; 3 ') being designed to bulk metal moulded parts and/or described washer arrangement is the plate (3a that belongs to bipolar plates; Part 3b), and the perforation (8,8 ') that is used for fluid transfer or gas medium is set at least one side of washer arrangement.
42. the method for production claim 27 or 41 described bipolar plates, wherein said bipolar plates have elastic washer device (7,7 '), described washer arrangement is made of metal and described bipolar plates (3; 3 ') being designed to bulk metal moulded parts and/or described washer arrangement is the plate (3a that belongs to bipolar plates; Part 3b) is characterized in that at first being provided with the hole on metallic plate, mechanical-moulded then plate with holes is with the production washer arrangement, and making becomes perforation in the above hole, at least one side of washer arrangement.
43. the method for production claim 27 or 41 described bipolar plates, described bipolar plates has the opening that is used for media discharge and medium supply and rubber-like and washer arrangement with the electro-chemical activity zone of sealed open and/or electrochemical cell is provided in some zone at least, and wherein washer arrangement and flow field are formed by metal sheet in a single manufacturing step.
Applications Claiming Priority (3)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE10248531A DE10248531B4 (en) | 2002-10-14 | 2002-10-14 | Fuel cell system and method for producing a bipolar plate contained in the fuel cell system |
| DE10248531.3 | 2002-10-14 | ||
| DE20308332.6 | 2003-05-22 |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1703795A CN1703795A (en) | 2005-11-30 |
| CN1292508C true CN1292508C (en) | 2006-12-27 |
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| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CNB2003801013314A Expired - Lifetime CN1292508C (en) | 2002-10-14 | 2003-10-14 | Electrochemical system |
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| CN (1) | CN1292508C (en) |
| DE (2) | DE10248531B4 (en) |
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Family Cites Families (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE10158772C1 (en) * | 2001-11-23 | 2003-06-26 | Reinz Dichtungs Gmbh & Co Kg | The fuel cell system |
-
2002
- 2002-10-14 DE DE10248531A patent/DE10248531B4/en not_active Expired - Lifetime
-
2003
- 2003-05-22 DE DE20308332U patent/DE20308332U1/en not_active Expired - Lifetime
- 2003-10-14 CN CNB2003801013314A patent/CN1292508C/en not_active Expired - Lifetime
Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107004885A (en) * | 2014-10-18 | 2017-08-01 | 莱茵兹密封垫有限公司 | Division board and electro-chemical systems |
| CN107004885B (en) * | 2014-10-18 | 2020-07-17 | 莱茵兹密封垫有限公司 | Separator and electrochemical system |
Also Published As
| Publication number | Publication date |
|---|---|
| CN1703795A (en) | 2005-11-30 |
| DE10248531A1 (en) | 2004-04-29 |
| DE20308332U1 (en) | 2004-02-12 |
| DE10248531B4 (en) | 2005-10-20 |
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