WO2023097587A1 - Procédé de préparation d'une plaque bipolaire pour pile à combustible électrochimique - Google Patents

Procédé de préparation d'une plaque bipolaire pour pile à combustible électrochimique Download PDF

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Publication number
WO2023097587A1
WO2023097587A1 PCT/CN2021/134945 CN2021134945W WO2023097587A1 WO 2023097587 A1 WO2023097587 A1 WO 2023097587A1 CN 2021134945 W CN2021134945 W CN 2021134945W WO 2023097587 A1 WO2023097587 A1 WO 2023097587A1
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WIPO (PCT)
Prior art keywords
bipolar plate
bipolar
substrate
thickness
flow channel
Prior art date
Application number
PCT/CN2021/134945
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English (en)
Chinese (zh)
Inventor
许哲荣
李志宏
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中兴电工机械股份有限公司
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Priority to PCT/CN2021/134945 priority Critical patent/WO2023097587A1/fr
Publication of WO2023097587A1 publication Critical patent/WO2023097587A1/fr

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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
    • 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
    • H01M8/0213—Gas-impermeable carbon-containing materials
    • 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

Definitions

  • Embodiments of the present invention relate to fuel cells, and in particular to bipolar plates for fuel cells.
  • Proton Exchange Membrane Fuel Cell is a relatively mature one among various fuel cells at present.
  • Proton exchange membrane fuel cells convert the chemical energy in fuel and air directly and continuously into electrical energy. Its basic principle is to pass fuel (such as hydrogen or methanol, etc.) on the anode side and oxidant (oxygen or air, etc.) on the cathode side, and make them electrochemically react under the action of the catalyst to generate water and electrical energy.
  • the bipolar plate (anode plate, cathode plate) in the proton exchange membrane fuel cell is mainly responsible for transporting the reaction gas to the catalyst reaction area for electrochemical reaction, and making the reaction gas evenly distributed on the membrane electrode group, and at the same time conducting the electrochemical reaction.
  • the bipolar plate also has the function of heat dissipation.
  • the material of the bipolar plate must have high electrical conductivity, good thermal conductivity and better corrosion resistance.
  • considering the processing of the flow channel on the bipolar plate it is also necessary to select the material of the bipolar plate. Consider its processing characteristics.
  • the most commonly used bipolar plate material is graphite, because its material properties meet the above characteristics, but its disadvantages are high material cost, poor mechanical strength, brittleness and limited processability. Due to the mechanical properties of graphite, most manufacturers use CNC (Computer Numerical Control) milling machines to process graphite bipolar plates.
  • the processed graphite bipolar plates are thick, bulky, and heavy (the weight of traditional graphite plates accounts for about 50% to 60% heavy) and other shortcomings, it is difficult to be used as a bipolar plate material for future miniaturization and lightweight fuel cells.
  • due to the complex machining process of CNC milling machines and the long machining cycle it is difficult to reduce the machining cost of graphite bipolar plates.
  • Metal materials also have high electrical conductivity and good thermal conductivity, and its excellent ductility enables it to be formed by stamping or hydraulic pressure, so that the thickness of the plate can be effectively reduced, so the use of metal bipolar plates can further reduce the battery stack
  • the volume and weight of the battery stack can increase the power density per unit volume and unit weight.
  • metal bipolar plates have good shock resistance, which can increase the competitiveness of fuel cell power systems applied to vehicles in the future.
  • the cost of metal is also lower than that of graphite, and the stamping method can also greatly shorten the production time of bipolar plates, thus reducing the cost of batteries in the mass production stage.
  • the disadvantage of metal bipolar plates is low corrosion resistance.
  • metal surface Under high temperature, high humidity and acidic fuel cell environments, the metal surface is prone to form a passivation layer due to corrosion and oxidation reactions, which in turn increases the contact resistance and reduces the power generation efficiency of the fuel cell. , On the other hand, metal ions may also damage the performance of MEA.
  • An embodiment of the present invention provides a bipolar plate for a fuel cell, which is formed by laminating substrates, wherein the substrate is formed of a flexible graphite plate, the density of the flexible graphite plate is 0.8-1.3g/cm 3 , and the carbon content> 98% and ash content ⁇ 2%, and based on the thickness of the substrate before pressing, the thickness compression rate of the bipolar plate is 40-50%.
  • the thickness deformation of the bipolar plate is 0.5-1 mm.
  • the flexible graphite plate has a sulfur content of ⁇ 1000 ppm and a chlorine content of ⁇ 50 ppm.
  • the density of the bipolar plates is 1-3 g/cm 3 .
  • the flow channel depth of the bipolar plate is ⁇ 1 mm.
  • the flow channel of the bipolar plate is a convoluted flow channel, a serpentine flow channel, an interdigitated flow channel, a grid-like flow channel or a parallel flow channel.
  • the embodiment of the present invention also provides a fuel cell, comprising: a proton exchange membrane; a pair of catalyst layers, respectively arranged on both sides of the proton exchange membrane; a pair of bipolar plates, respectively arranged on the outside of the catalyst layer, the proton exchange membrane And the catalyst layer is clamped in the middle, wherein the bipolar plate is the bipolar plate of any example in the above-mentioned embodiments.
  • An embodiment of the present invention further provides a method for manufacturing a bipolar plate for a fuel cell, including: a die cutting step, cutting the soft graphite plate into a substrate; a matching step, placing the substrate in a mold; pressing step, pressing the mold on which the substrate is placed; and a demolding step, separating the pressed substrate from the mold to obtain a bipolar plate, wherein the density of the soft graphite plate is 0.8-1.3g/cm 3 , carbon The content is >98% and the ash content is ⁇ 2%, and based on the thickness of the substrate before lamination, the thickness compression rate of the bipolar plate is 40-50%.
  • the mold has a draft angle of 1-10°.
  • the pressing weight of the pressing step is 300-1500 kg/cm 2 .
  • the pressing step is performed at room temperature.
  • the duration of the pressing step is 0.05-3 minutes.
  • 1A-1E are partial schematic diagrams illustrating flow channels of a bipolar plate, according to some embodiments.
  • FIG. 2 is a partial schematic diagram illustrating a fuel cell, according to some embodiments.
  • FIG. 3A is a schematic diagram illustrating a substrate placed in a mold and pressed together, according to some embodiments.
  • FIG. 3B is a schematic diagram illustrating a bipolar plate obtained after demolding, according to some embodiments.
  • 4A-4B are partial side views illustrating a mold, according to some embodiments.
  • first element is formed on a second element
  • it may include an embodiment in which the first and second elements are in direct contact, or may include an additional element formed between the first and second elements , so that they are not in direct contact with the example.
  • embodiments of the present invention may repeat reference numerals or letters in various examples. This repetition is for the purpose of brevity and clarity and not to show the relationship between the different embodiments or configurations discussed.
  • the disclosure provides a bipolar plate for a fuel cell, the main feature of which is that the bipolar plate is formed by direct pressing of a soft graphite plate, which can provide high-durability fuel in a low-cost and high-efficiency manner Battery bipolar plates.
  • the "soft graphite plate” referred to in this case refers to a graphite plate with a density of 0.8-1.3 g/cm 3 , a tensile strength of 40-50 kg/cm 2 , a carbon content >98%, and an ash content ⁇ 2%.
  • the flexible graphite plate may be made of expanded graphite material, for example.
  • the expanded graphite material can be, for example, made of natural flake graphite through intercalation treatment, water washing, drying, and high-temperature expansion.
  • the flexible graphite plate has a density of about 0.8-1.3 g/cm 3 (eg, 0.9-1 g/cm 3 , 0.95-1.2 g/cm 3 ).
  • the flexible graphite plate has a carbon content >98% (eg >98.5%, >99%, >99.5%) and an ash content ⁇ 2% (eg ⁇ 1.5%, ⁇ 1%, ⁇ 0.5%).
  • the high carbon content of the flexible graphite plate achieves high thermal conductivity and electrical conductivity, so as to meet the needs of the electrochemical reaction of the fuel cell.
  • the flexible graphite sheet is cut to form the substrate.
  • the flexible graphite plate does not contain resin, so the bipolar plate formed by directly pressing the cut substrates can maintain the characteristic of high electrical conductivity.
  • the tensile strength of the flexible graphite sheet is about 40-50 kg/cm 2 (eg, 42-45 kg/cm 2 , 43-48 kg/cm 2 ).
  • the compressibility of the flexible graphite sheet is >40% (eg >50%, >60%).
  • the thickness compression rate of the bipolar plate is 40-50% (such as 42-45%, 43-48%), that is, based on the thickness of the substrate before lamination
  • the thickness of the bipolar plate formed after pressing is reduced by 40-50%.
  • the thickness of the substrate is the maximum thickness of the entire substrate
  • the thickness of the bipolar plate is the maximum thickness of the entire bipolar plate.
  • the thickness deformation of the bipolar plate is 0.5-1 mm (eg, 0.6-0.9 mm, 0.7-0.8 mm).
  • soft graphite needs to be impregnated with resin to obtain higher mechanical strength.
  • the soft graphite can be formed by controlling the thickness compressibility of the bipolar plate and/or the thickness deformation of the bipolar plate.
  • the bipolar plate remains unbroken. If the thickness compressibility of the bipolar plate is too low, the strength of the bipolar plate will be too low and the impedance value will be too high. If the thickness compression rate of the bipolar plate is too high, it will increase the difficulty of demolding the bipolar plate, and it is easy to break during the compression process.
  • the density of the bipolar plates is about 1-3 g/cm 3 (eg, 1.2-2.5 g/cm 3 , 1.6-2 g/cm 3 ).
  • the sulfur content of the flexible graphite plate ⁇ 1000ppm and the chlorine content ⁇ 50ppm by controlling the sulfur content and the chlorine content in the flexible graphite plate, the impact on the catalyst in the fuel cell can be suppressed, thereby improving fuel efficiency. battery durability.
  • a bipolar plate 10 has flow channels 12 , flow channel inlets 14 , flow channel outlets 16 , and the like.
  • the flow channel 12 can be, for example, a convoluted flow channel (as shown in Figure 1A), a serpentine flow channel (as shown in Figure 1B), an interdigitated flow channel (as shown in Figure 1C), a grid-shaped flow channel (as shown in Figure 1D) or a parallel flow channel Road (as shown in Figure 1E) and so on.
  • the channel depth of the bipolar plate 10 is about ⁇ 1 mm (eg ⁇ 0.8 mm, ⁇ 0.5 mm).
  • the bipolar plate of the present application can be used as a bipolar plate (anode plate and/or cathode plate) of a fuel cell.
  • the flow channels on the bipolar plate of the present invention can be used as gas flow channels (such as hydrogen, air, etc.) and/or liquid flow channels (such as cooling liquid or methanol, etc.).
  • bipolar plates may have flow channels on both sides.
  • a bipolar plate may have flow channels on a single face.
  • FIG. 2 is a partial schematic diagram of a fuel cell 100 using a bipolar plate of the present invention.
  • the fuel cell 100 may be composed of multiple single cells connected in series.
  • fuel cell 100 includes proton exchange membrane 20 .
  • the fuel cell 100 includes a pair of catalyst layers (an anode catalyst layer 30 a and a cathode catalyst layer 30 b ), respectively disposed on two sides of the proton exchange membrane 20 .
  • the fuel cell 100 includes a pair of bipolar plates (anode plate 10a and cathode plate 10b), which are respectively arranged on the outside of the anode catalyst layer 30a and the cathode catalyst layer 30b, and the proton exchange membrane 20, the anode catalyst layer 30a And the cathode catalyst layer 30b is sandwiched in the middle.
  • the hydrogen enters the channel 12a from the gas inlet of the anode plate 10a, and diffuses to the anode catalyst layer 30a through the gas diffusion layer (not shown).
  • the air enters the channel 12b from the air inlet of the cathode plate 10b, and diffuses to the cathode catalyst layer 30b through a gas diffusion layer (not shown).
  • the anode catalyst layer 30a Through the action of the anode catalyst layer 30a, the hydrogen atoms at the anode are decomposed into two hydrogen protons and two electrons, among which the protons are "attracted" to the other side of the proton exchange membrane 20, and the electrons reach the cathode through an external circuit to form a current .
  • the cathode catalyst layer 30b hydrogen protons, oxygen and electrons react to form water molecules.
  • the anode catalyst layer 30a may include, for example, Pt, Ru, Ni, or the like.
  • the cathode catalyst layer 30b may include, for example, Pt, Ni, or the like.
  • the anode plate 10a and the cathode plate 10b of the fuel cell 100 may further have a flow channel 13a and a flow channel 13b respectively.
  • the flow channel 13a and the flow channel 13b are cooling liquid flow channels.
  • fuel cells have better transfer efficiency than conventional internal combustion engines, about 50% of the energy is still dissipated as waste heat. Therefore, the flow channels 13a and 13b can make the flow distribution of the cooling liquid on the surface of the anode plate 10a and the cathode plate 10b respectively uniform, so as to achieve the effect of uniform heat dissipation.
  • the fuel cell 100 may further include collector plates, end plates, sealing layers and other existing components, which are not described in detail here for simplicity.
  • the fabrication of the bipolar plates includes a die cutting step, cutting the flexible graphite plates into substrates.
  • the soft graphite plate a commercially available soft graphite plate can be directly used.
  • the size of the flexible graphite plate before cutting can be, for example, about 20-40 cm long (for example, about 23-35 cm, 25-30 cm), and about 20-40 cm wide (for example, about 23-35 cm, 25-30 cm ), about 0.3-3cm high (for example about 1-2.8cm, 1.5-2.5cm).
  • the size of the cut substrate can be set according to requirements, for example, it can be about 3-30cm long (for example, about 10-28cm, 15-20cm), and about 3-30cm wide (for example, about 10-28cm, 15-20cm) , about 0.3-3cm in height (for example about 1-2.8cm, 1.5-2.5cm).
  • the runner outlet and runner inlet gas outlet and inlet and/or coolant outlet and inlet
  • the position and location of the cut runner outlet and runner inlet can be set according to actual product requirements. size.
  • a matching step is performed after the die cutting step.
  • the substrate 50 is placed in the mold 300 , wherein the thickness of the substrate 50 is d1 .
  • a suitable mold 300 can be manufactured and selected according to requirements. By setting the texture on the mold 300, the shape of the flow path of the bipolar plate formed after lamination can be determined, and the bipolar plate can be set by the outer frame of the mold. board size.
  • a pressing step is performed after the matching step, and the mold 300 on which the substrate 50 is placed is subjected to pressing. Through the application of pressure, the substrate 50 is deformed along with the pattern of the mold 300 to form a shape with a specific flow channel.
  • the pressing weight of the pressing step is about 300-1500 kg/cm 2 (eg, 500-1300 kg/cm 2 , 650-1200 kg/cm 2 , 700-1000 kg/cm 2 ). By controlling the pressing weight within this range, the thickness compressibility and/or thickness deformation of the bipolar plate can be controlled, so that the bipolar plate has sufficient rigidity.
  • the pressing step is performed at normal temperature and the duration of the pressing step is about 0.05-3 minutes (eg, 1-2.5 minutes, 1.5-2.3 minutes).
  • the demoulding step is performed after the pressing step, and the pressed substrate 50 is separated from the mold 300 by vigorously hitting the demoulding base downward, so as to obtain the bipolar plate 10 having the flow channel 12 and the flow channel 13 , as shown in FIG. 3B , wherein the maximum thickness of the bipolar plate 10 as a whole is d2.
  • the entire manufacturing process takes no more than 5 minutes (such as 1-4 minutes, 2-3 minutes), which greatly shortens the processing time of the bipolar plate.
  • the combined pressure in pounds and the thickness deformation of the bipolar plate have a relationship as shown in Table 1.
  • the substrate used in the embodiment has a length of about 5-25 cm, a width of about 5-25 cm, and a height of about 0.5-2 cm, and the pressing time is 1-2 min.
  • the mold has a draft angle of 1-10°.
  • the mold has a lead/rounded design.
  • the draft angle is the slope of the mold, which is the slope designed on both sides of the cavity for the convenience of mold release.
  • the draft angle In order to allow the molded product to be ejected from the mold smoothly, the draft angle must be set on the wall in the same direction as the opening and closing of the mold to facilitate demoulding. Since the soft graphite plate is easier to stick to the mold, by setting the draft angle of the mold in the range of 1-10°, the friction force during demolding can be reduced, and the bipolar plate can be completely separated.
  • the mold with traditional right-angle design does not have a draft angle, which makes it difficult to demould later.
  • Figure 4A is a partial side view of mold 300, according to some embodiments.
  • the angle between the side wall of the mold 300 and its vertical direction is the draft angle s.
  • the mold 300 with the draft angle s can reduce the friction between the mold and the material to be pressed in the vertical direction during demoulding, so that the material to be pressed can be released from the mold more easily.
  • the draft angle s may be about 1° to about 10° (eg, about 2° to 8°, about 3° to 6°).
  • the mold 300 in addition to the draft angle, the mold 300 also has a lead/round corner design, as shown in FIG. 4B , which further reduces friction.
  • various physical inspections can be performed to confirm that the finished specification of the bipolar plate meets the requirements of the product.
  • a thickness gauge can be used to detect the thickness of the bipolar plate;
  • a depth gauge can be used to detect the depth of the flow channel of the bipolar plate;
  • a caliper can be used to detect the length of the bipolar plate.
  • bipolar plates may be bonded for gas leak detection.
  • an impedance test and an electrical test may be performed on the bipolar plate.
  • the material cost of a pure graphite bipolar plate costs thousands of yuan, while the material cost of a bipolar plate made of soft graphite plate is only tens of yuan, saving at least 90% of the material. cost.
  • the bipolar plate made of flexible graphite plate in this case can pass the airtight test and electrical test to prove that its material will not affect the performance of the fuel cell. That is to say, the bipolar plate formed by pressing the soft graphite plate in this application can save the manufacturing cost and shorten the manufacturing time without reducing the performance of the fuel cell.
  • the metal bipolar plate can be processed quickly through the stamping process, and the cost of the metal is lower than that of graphite, but in the environment of high temperature, high humidity and acidity of the fuel, the metal bipolar plate is prone to oxidation, and additional processing is required ( Plating) anti-oxidation surface treatment, so its durability is low.
  • the soft graphite plate used in this case will not have the problem of oxidation, and is more suitable for long-term use products.
  • the bipolar plate made of soft graphite plate in this case has the advantages of low cost, fast processing, and good durability.

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Abstract

La présente invention concerne une plaque bipolaire pour une pile à combustible. La plaque bipolaire est formée par stratification d'un substrat. Le substrat est constitué d'une plaque de graphite souple. La plaque de graphite souple présente une densité de 0,8 à 1,3 g/cm3, une teneur en carbone supérieure à 98 % et une teneur en cendres inférieure à 2 % ; et sur la base de l'épaisseur du substrat avant stratification, le rapport de compression d'épaisseur de la plaque bipolaire est de 40 à 50 %.
PCT/CN2021/134945 2021-12-02 2021-12-02 Procédé de préparation d'une plaque bipolaire pour pile à combustible électrochimique WO2023097587A1 (fr)

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PCT/CN2021/134945 WO2023097587A1 (fr) 2021-12-02 2021-12-02 Procédé de préparation d'une plaque bipolaire pour pile à combustible électrochimique

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PCT/CN2021/134945 WO2023097587A1 (fr) 2021-12-02 2021-12-02 Procédé de préparation d'une plaque bipolaire pour pile à combustible électrochimique

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Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2000021422A (ja) * 1998-06-30 2000-01-21 Toshiba Corp 燃料電池用セパレータの製造方法及び燃料電池用セパレータ
JP3054600B2 (ja) * 1997-03-14 2000-06-19 株式会社東芝 固体高分子電解質燃料電池用セパレータおよびその製造方法
US20020127390A1 (en) * 2000-12-07 2002-09-12 Oswin Ottinger Acrylic resin-impregnated bodies formed of expanded graphite, process for producing such bodies and sealing elements, fuel cell components and heat-conducting elements formed of the bodies
US20020174782A1 (en) * 2001-05-11 2002-11-28 Klug Jeremy H. Process to reduce warping of graphite articles
US20090061191A1 (en) * 2007-09-04 2009-03-05 Aruna Zhamu Recompressed exfoliated graphite articles
CN111689491A (zh) * 2020-05-29 2020-09-22 浙江国泰萧星密封材料股份有限公司 用于氢燃料电池双极板的柔性石墨制造工艺

Patent Citations (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP3054600B2 (ja) * 1997-03-14 2000-06-19 株式会社東芝 固体高分子電解質燃料電池用セパレータおよびその製造方法
JP2000021422A (ja) * 1998-06-30 2000-01-21 Toshiba Corp 燃料電池用セパレータの製造方法及び燃料電池用セパレータ
US20020127390A1 (en) * 2000-12-07 2002-09-12 Oswin Ottinger Acrylic resin-impregnated bodies formed of expanded graphite, process for producing such bodies and sealing elements, fuel cell components and heat-conducting elements formed of the bodies
US20020174782A1 (en) * 2001-05-11 2002-11-28 Klug Jeremy H. Process to reduce warping of graphite articles
US20090061191A1 (en) * 2007-09-04 2009-03-05 Aruna Zhamu Recompressed exfoliated graphite articles
CN111689491A (zh) * 2020-05-29 2020-09-22 浙江国泰萧星密封材料股份有限公司 用于氢燃料电池双极板的柔性石墨制造工艺

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