• 专利附录
  • 专利说明
  • 权利要求
  • 类似技术
  • 同族专利
  • 引用文献
  • 法律状态
  • 优先权
    • 专利摘要:
    In a fuel cell assembly typically comprised of a plurality of cells each having an electrolyte layer 2, a pair of gas diffusion electrode layers 3, 4 and a pair of diffuser plates 5, the electrolyte layer 2 ) Has a frame 21 and an electrolyte 22 held in the frame; The flow distribution plate and frame are made of a material having similar thermal expansion properties to avoid the occurrence of thermal stress between the frame of the electrolyte layer and the corresponding flow distribution plate, and the durability of the various materials is ensured. By joining each flow distribution plate along its periphery with a corresponding frame and anodic bonding or bonding agent, the need for a sealing arrangement, such as a gasket split clamping arrangement, is eliminated, which is an intensive design of the assembly. Contribute to.
    公开号:KR20020093978A
    申请号:KR1020027014888
    申请日:2001-05-08
    公开日:2002-12-16
    发明作者:사사하라준；구리야마나리아키；구보타다다히로；이소가이유지；이상준존
    申请人:혼다 기켄 고교 가부시키가이샤；스탠포드 유니버시티；
    IPC主号:
    专利说明:

    Fuel cell assembly
    [2] The fuel cell has an electrolyte layer and a pair of electrodes disposed on one side of the electrolyte layer, and the electricity is supplied with the aid of a catalyst through an electrochemical reaction between a fuel gas such as hydrogen and alcohol and an oxidizing gas such as oxygen and air. And it is supplied to the corresponding electrode. Depending on the electrolyte material used as the electrolyte layer, the fuel cell may be referred to as phosphoric acid type or solid polymer type or molten carbonate type.
    [3] In particular, solid polymer electrolyte (SPE) type fuel cells using ion-exchange resin membranes for the electrolyte layer have high density, low operating temperatures (100 degrees C or less) and high It is considered very promising because of its efficiency.
    [4] SPE is commonly used as an ion exchange resin membrane for perfluorocarbonsulfonic acid (Nafion trade name), phenolsulfonic acid, polyethylenesulfonic acid and polytrifluorosulfo. It is made from polytrifluorosulfonic acid and the like. A porous carbon sheet impregnated with a catalyst such as platinum powder is placed on each side of the ion exchange resin membrane for use as a gas diffusion electrode layer. This assembly is called a membrane-electrode assembly (MEA). The fuel cell may be formed by defining a fuel gas passage on one side of the MEA and defining an oxidizing gas passage on the other side of the MEA by using a flow distribution plate (separators).
    [5] Typically, such fuel cells are stacked and the flow distribution plates are shared by adjacent fuel cells in the same stack. In forming such a stack, it is necessary to seal a passage defined on the surface of the MEA from the outside. Traditionally, gaskets are disposed around the interface between adjacent pairs of MEAs and distribution plates. The contact area between the MEA and the gas diffusion electrode is ensured by pressing them together and applying an external force, which is usually by the aid of a suitable fixture. The required electrical connection between the gas diffusion electrode and the electrode terminal connected to the external circuit is also ensured by pressing them together and applying an external force.
    [6] However, since the MEA changes its volume depending on the amount of moisture and the temperature of the SPE, the external force exerted by the fixture inevitably changes, which may worsen the sealing ability of the assembly. The SPE may be surrounded by the frame to stabilize the shape of the SPE, but since the frame and the flow distribution plate thermally expand and individually contact, the external force exerted by the fixture still changes. The change in external force in this case causes stress on the various members, which worsens the durability of the various members of the assembly.
    [7] Packaging and / or arrangement to ensure such controlled pressure and the required sealing performance tend to be large, which has hampered the intensive design of the fuel cell assembly. Moreover, even with highly sophisticated arrangements to ensure sealing performance, it was very difficult to maintain the required sealing performance for extended periods of time due to irregular thermal expansion and contraction of various components.
    [1] This application claims the benefit of US Provisional Application Nos. 60 / 202,827, filed May 8, 2000 and 60 / 242,136, filed October 23, 2000, both of which are incorporated herein by reference. The present invention typically includes a plurality of fuel cells, each comprising an electrolyte layer, a pair of gas diffusion electrode layers disposed on one side of the electrolyte layer, and a gas diffusion electrode layer disposed on one of the outer sides of the gas diffusion electrode layer. A fuel cell assembly having a pair of flow distribution plates defining a passage of fuel gas and oxidizing gas in cooperation with opposing sides of the same.
    [16] The invention is now described with reference to the accompanying drawings.
    [17] 1 is a partially enlarged perspective view of a fuel cell assembly implementing the present invention;
    [18] 2A is a cross-sectional view taken along section IIa-IIa of FIG. 1,
    [19] FIG. 2B is a cross-sectional view taken along section IIb-IIb of FIG. 1;
    [20] 3A-3C are cross-sectional views of the electrolyte layer at different stages of the manufacturing process,
    [21] 4A-4C are cross-sectional views of flow distribution plates at another stage of the manufacturing process.
    [8] In view of such problems of the prior art, the main object of the present invention is to provide a fuel cell assembly capable of ensuring good sealing under all conditions.
    [9] It is a second object of the present invention to provide a fuel cell assembly capable of ensuring reliable electrical contact between an electrode terminal and a gas diffusion electrode.
    [10] It is a third object of the present invention to provide a fuel cell assembly which is highly compact and at the same time efficient.
    [11] It is a fourth object of the present invention to provide a fuel cell assembly that is easy to manufacture.
    [12] According to the invention, the object is to provide an electrolyte layer, a pair of gas diffusion electrode layers interposed between the electrolyte layers between them, and a pair of flow distribution plates defining a passage of fuel and oxidant in contact with the gas diffusion electrode layer. A fuel cell assembly comprising at least one cell comprising: an electrolyte layer comprising a frame and an electrolyte retained in the frame, and each flow distribution plate and the corresponding frame having its periphery in order to obtain an airtight cavity therebetween. It is achieved by providing a fuel cell assembly characterized in that coupled together. Each flow distribution plate and the corresponding frame may be joined by anodical bonding, diffusion bonding, welding, brazing and bonding.
    [13] This allows the flow distribution plate and frame to be combined with the required sealing capacity without requiring any clamping arrangement, any arrangement that depends on fixtures or external forces.
    [14] In particular, if the flow distribution plate and frame are made of a material having similar thermal expansion properties, even if the assembly is subject to changes in temperature, because the frame and flow distribution plate for the electrolyte layer expand and contract in a similar manner, Stresses inside the assembly can also be avoided. This contributes to the protection of the assembly's sealing performance and to the improvement of the assembly's durability over extended periods of time and even under extreme conditions.
    [15] Preferably, both the flow diffuser plate and the frame of the electrolyte layer can be made from a silicon wafer suitable for fine work processes. According to a preferred embodiment of the present invention, the flow distribution plate and the frame of the electrolyte layer are joined along their periphery by annodic bonding or bonding agent. This eliminates the need for a gasket or clamping arrangement and increases the reliability of the assembly over extended periods of time and under extreme conditions while simplifying the structure of the assembly.
    [22] 1 illustrates the structure of one component of a fuel cell assembly implementing the present invention. Indeed, a plurality of cells are formed in a stack and a large number of such stacks are connected in series and / or in parallel, and a fuel composed of an improved alcohol, hydrogen gas or the like is provided in each fuel cell stack with an oxidizing gas such as air. Supplied with.
    [23] Referring also to FIGS. 2A and 2B, each fuel cell 1 has a central electrolyte layer 2, a pair of gas diffusion electrode layers 3 (4) disposed on one side of the central electrolyte layer 2 (FIG. 2A). And 2b) and a pair of flow distribution plates 5 disposed on one outer side of the gas diffusion electrode layer 3 and 4. The outer side of each flow distribution plate 5 is formed similarly to its inner side for use as the flow distribution plate of an adjacent fuel cell.
    [24] The electrolyte layer 2 has a solid polymer electrolyte (SPE) 22 filled into a rectangle through holes 21b defined between the grid frame 21 and the adjacent bars 21a of the grid frame 21. SPE (22) is a perfluorocarbonsulfonic acid (Nafion (trade name)), phenolsulfonic acid, polyethylenesulfonic acid and polytrifluorosulfonic acid ) And so on.
    [25] The grid frame 21 is formed by etching or otherwise processing a silicon wafer and is provided with a rectangular, annular fringe portion and a rectangular grid region defined within the annular fringe portion. Each bar 21a in the grid area of the grid frame 21 has a projection 21c in its middle portion so as to project into the middle portion of the corresponding through hole 21b best shown in FIGS. 2A and 2B. ) Is provided.
    [26] The protrusion 21c is shaped like a ridge that extends along the length of the bar 21a and provides a narrower middle portion in each through hole 21b. The protrusion 21c helps to hold the SPE 22 in each passage hole 21b.
    [27] Such protrusions may be conveniently formed while forming the grid frame 21. 3A-3C show the process of forming the electrolyte layer 2. Above all, a suitably patterned photoresist layer 13, 14 is disposed on each side of the silicon wafer used as the material of the grid frame 21 shown in FIG. 3A.
    [28] Anisotropic etching is performed from both sides of the wafer shown in Fig. 3B, which produces a plurality of through holes 21b, each of which is narrowed in the center portion by the protrusions 21c. Then, the SPE 22 is filled in each of the through holes 21b to define a planar surface that is substantially horizontal on each side of the electrolyte layer 2.
    [29] In this embodiment, rectangular through holes 23a, 23b, 24a and 24b are formed at each corner of the fringe of the grid frame 21. One of the diagonally opposed pairs of these through holes 23a and 23b is used as the inlet and outlet of the fuel gas. The remaining opposing pairs of these through holes 24a and 24b serve as the inlet and outlet of the oxidizing gas.
    [30] Each flow distribution plate 5 also has a rectangular shape which is formed by processing a silicon wafer and is substantially coincident. A rectangular recess 51 or 52 having a flat bottom is formed at the center on each side of the flow distribution plate 5, and a plurality of protrusions 53 or 54 each having the shape of a cut pyramid are formed at the flat bottom. do. The surface of the recesses and protrusions is coated with a gold plate layer which is used as the electrode terminal layer 55 or 56 by suitable means for electrically connecting the gas diffusion electrode layers 3 and 4 to the circuitry.
    [31] 4A-4C show the process of forming each flow distribution plate 5. A suitably patterned photoresist layer 15, 16 is formed on each side of the silicon wafer shown in FIG. The wafer is etched from both sides to form recesses 51 and 52 and protrusions 53 and 54 at the same time as shown in FIG. 4B. The distribution plate 5 of the upper end or lower end of each fuel cell stack may be provided with recesses and protrusions only inside thereof. Thus, electrode terminal layers 55 and 56 are formed over the surfaces of recesses 51 and 52 and protrusions 53 and 54 as shown in FIG. 4C.
    [32] The distribution plate 5 coincides with the grid frame 21 and thus has a rectangular shape. Rectangular through holes 57a, 57b, 58a or 58b are formed at each corner of its fringe. One of the diagonally opposite pairs of these through holes 57a and 57b serves as an inlet or outlet of fuel gas. The remaining opposing pairs of these through holes 58a and 58b serve as inlets and outlets for the oxidizing gas. As shown in Fig. 1, the grooves 59a and 59b formed in the fringes communicate with the through holes 58a and 58b for the oxidizing gas and similar grooves 60a and 60b form the recesses 52. It communicates with the passage holes 57a and 57b for the fuel gas.
    [33] The gas diffusion electrode layers 3 and 4 are each composed of carbon sheets 3a or 4b having layers of platinum catalysts 3b and 4b mixed with SPE formed on their sides towards the electrolyte layer 2.
    [34] In this way, in each fuel cell, a pair of flow distribution plates 5 are arranged on one side of the electrolyte layer 2 via the gas diffusion electrode layer 3 or 4, and this component is used to cover the portion surrounding the recess. Therefore, they are bonded by anodic bonding. Thus, the plurality of narrow passages 11 is limited to one of the central recesses 52 of each electrolyte layer 2 for fuel gas, and the plurality of similar narrow passages 10 are the electrode layers 2 for the oxidizing gas. Is limited to the other one of the central recesses 51. Each protrusion is covered by a gold plate layer that is used substantially as an electrode terminal, and lightly pushes the gas diffusion electrode layer 3 or 4 against the frame grid 21 of the electrolyte layer 2. Thus, each gas diffusion electrode layer 3 or 4 is connected to the corresponding distribution plate 5 electrically through many protrusions in parallel relationship, and a reliable electrical connection between the electrolyte layer 2 and the external circuit can be made. have.
    [35] Bonding between the grid frame 21 and the distribution plate 5 can be achieved by many different methods. Preferably, annodic bonding is used as described below. The hard frame made from the electrode layer 9 and the heat resistant layer 8 and for example Pyrex glass (trade name) is a grid frame of the electrolyte layer 2 on one side thereof by sputtering. Along the peripheral surface of 21 is formed, a similar electrode layer 9 is formed along the periphery of the opposing surface of the distribution plate 5. Then, while the assembly is heated to about 400 degrees Celsius, the temperature at which sodium ions are highly fluid, an electric field is generated in the assembly to transport the ions. In the fuel cell assembly of the present invention, if the electrolyte consists of a solid polymer, heating the entire assembly to 400 degrees Celsius can damage the solid electrolyte. Thus, according to this embodiment, a heater (not shown) is arranged below the electrode layer 9 to selectively heat only the peripheral portion of the flow distribution plate. The heater may consist of polycrystalline sandwiched between insulating layers such as Si 3 N 4 . If the electrode terminal layers 55 and 56 extend under the heater, the thermal efficiency of the heater is deteriorated. Thus, it is desirable to remove the electrode terminal layers 55 and 56 from the bottom of the heater.
    [36] The grid frame 21 and the distribution plate 5 are arranged one above the other and are compressed at a pressure of 100 gf / cm 2 to 2,000 gf / cm 2 . Current is passed through the polycrystalline silicon heater to heat the locally bonded portion to around 400 degrees Celsius. At the same time, a voltage of about 100 to 500 volts is applied between 10 and 30 minutes between the electrode layer 9 of the grid frame 21 and the electrode layer 9 of the distribution plate 5.
    [37] Alternatively, a binder may be used to attach the grid frame 21 and the distribution plate 5 together. In either case, the need for any sealing arrangement or clamping arrangement can be eliminated to achieve the desired sealing capability, which allows for intensive design of the fuel cell assembly.
    [38] As fuel gas and oxidizing gas (air) pass through this fuel cell 1, an electrochemical reaction takes place with the help of a platinum catalyst and a voltage is applied between the electrode terminal layers 55 and 56. A large number of these fuel cells are stacked so that the desired voltage can be obtained.
    [39] Although the fuels and oxidants for the fuel cells described herein are composed of gases they also contain liquids.
    [40] Although the invention has been described using its preferred embodiments, it is apparent to those skilled in the art that various alternatives and modifications are possible without departing from the scope of the invention set forth in the appended claims.
    [41] The invention can be used in the field of fuel cells.
    权利要求:
    Claims (7)
    [1" claim-type="Currently amended] Electrolyte layer (2), a pair of gas diffusion electrode layers (3, 4) interposed between the electrolyte layer and a pair of passages (10, 11) defining a passage (10, 11) for fuel and oxidant gas in contact with the gas diffusion electrode layer A fuel cell assembly comprising at least one cell having a flow distribution plate 5,
    The electrolyte layer 2 has a frame 21 and an electrolyte 22 held between the frames;
    Each flow distribution plate and corresponding frame are coupled along its periphery to obtain a tightly sealed cavity therebetween.
    [2" claim-type="Currently amended] The method of claim 1,
    And a frame corresponding to each flow distribution plate is joined by anodic bonding.
    [3" claim-type="Currently amended] The method of claim 1,
    And a frame corresponding to each flow distribution plate is joined by a binder.
    [4" claim-type="Currently amended] Electrolyte layer (2), a pair of gas diffusion electrode layers (3, 4) interposed between the electrolyte layer and a pair of passages (10, 11) defining a passage (10, 11) for fuel and oxidant gas in contact with the gas diffusion electrode layer A fuel cell assembly comprising at least one cell having a flow distribution plate 5,
    The electrolyte layer 2 has a frame 21 and an electrolyte 22 held between the frames;
    And the flow distribution plate and frame are made of a material having a similar coefficient of thermal expansion.
    [5" claim-type="Currently amended] The method of claim 4, wherein
    Each flow distribution plate and corresponding frame are joined by anodical bonding along their periphery to obtain a tightly sealed cavity therebetween.
    [6" claim-type="Currently amended] The method of claim 4, wherein
    Each flow distribution plate and the corresponding frame are joined by a binder along its periphery to obtain a tightly sealed cavity therebetween.
    [7" claim-type="Currently amended] The method of claim 4, wherein
    A fuel cell assembly, wherein the flow distribution plate and frame are made of a silicon substrate.
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    引用文献:
    公开号 | 申请日 | 公开日 | 申请人 | 专利标题
    法律状态:
    2000-05-08|Priority to US20282700P
    2000-05-08|Priority to US60/202,827
    2000-10-23|Priority to US24213600P
    2000-10-23|Priority to US60/242,136
    2001-05-08|Application filed by 혼다 기켄 고교 가부시키가이샤, 스탠포드 유니버시티
    2002-12-16|Publication of KR20020093978A
    2005-11-24|Application granted
    2005-11-24|Publication of KR100531049B1
    优先权:
    申请号 | 申请日 | 专利标题
    US20282700P| true| 2000-05-08|2000-05-08|
    US60/202,827|2000-05-08|
    US24213600P| true| 2000-10-23|2000-10-23|
    US60/242,136|2000-10-23|
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