CN112786911A - Bipolar plate and electrode frame integrated structure and preparation method and application thereof - Google Patents
Bipolar plate and electrode frame integrated structure and preparation method and application thereof Download PDFInfo
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- CN112786911A CN112786911A CN202110063172.3A CN202110063172A CN112786911A CN 112786911 A CN112786911 A CN 112786911A CN 202110063172 A CN202110063172 A CN 202110063172A CN 112786911 A CN112786911 A CN 112786911A
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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
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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
- H01M8/0221—Organic resins; Organic polymers
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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
- H01M8/0223—Composites
- H01M8/0228—Composites in the form of layered or coated products
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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
- H01M8/18—Regenerative fuel cells, e.g. redox flow batteries or secondary fuel cells
- H01M8/184—Regeneration by electrochemical means
- H01M8/188—Regeneration by electrochemical means by recharging of redox couples containing fluids; Redox flow type batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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Abstract
The invention belongs to the field of flow batteries, and discloses a bipolar plate and electrode frame integrated structure, and a preparation method and application thereof. The method comprises the following steps: selecting a plastic plate, cutting the plastic plate into the size of an electrode frame, manufacturing a substrate, roughening the bottom of a groove of the substrate, and coating a layer of conductive solution to form a conductive liquid film on the surface of the substrate; and spraying a carbon material coating with a certain thickness by using an electrostatic spraying mode to prepare an integrated prefabricated plate of the bipolar plate and the electrode frame, placing the prefabricated plate in a vacuum drying box, drying to constant weight, placing the prefabricated plate on a hot press, performing hot pressing to enable the carbon material coating to be tightly and firmly combined with the plastic plate, cooling, and connecting the carbon material coatings at the extending ports of the grooves on the two sides of the plate by using a conductive material to obtain the integrated structure of the bipolar plate and the electrode frame, wherein the integrated structure simultaneously has high conductivity and strong mechanical property. The invention has good liquid resistance effect, reduces the thickness of the electrode and reduces the internal resistance of the electrode.
Description
Technical Field
The invention belongs to the field of flow batteries, and relates to a bipolar plate and electrode frame integrated structure, and a preparation method and application thereof.
Background
The bipolar plate is a key component for assembling fuel cell single cells into a cell stack in series, has the functions of separating reaction gas, guiding the fuel reaction gas into the fuel cell through a flow field, collecting and conducting current, supporting a membrane electrode, and simultaneously playing a role in heat dissipation and water drainage of the whole cell system. In the prior art, graphite and metal plates are widely used as materials for manufacturing bipolar plates. The metal bipolar plate has the advantages of high conductivity, good mechanical strength and low price, can process a gas flow field and a cooling water flow field through stamping, can be processed into a thin plate, reduces the thickness and the weight of the bipolar plate, and the like, and gradually becomes the mainstream of the bipolar plate. However, the metal is inevitably dissolved and corroded at the high temperature and electrochemical corrosion of the fuel cell. In particular, metal ions penetrate into the proton exchange membrane, which can lead to membrane poisoning. Meanwhile, the bipolar plate increases contact resistance due to the corrosion layer, and reduces the performance of the fuel cell. Therefore, the surface of the metal bipolar plate must be modified in the prior art.
Two typical technological methods are used for modifying the surface of the bipolar plate, wherein the first method comprises the steps of firstly carrying out surface modification on a stamped unipolar plate thin plate, electroplating precious metal or Physical Vapor Deposition (PVD) carbide, and finally welding the unipolar plate thin plate into the bipolar plate. The method has the disadvantages that the surface modification layer is damaged at the welding part, so that the welding seam can only be in the non-working area of the bipolar plate seal, the welding part is few, and the resistance of the bipolar plate is multiplied; the second method is to weld the unipolar plate into the bipolar plate, and weld the bipolar plate in the working area to increase the welding position and reduce the resistance of the bipolar plate, and then to electroplate noble metal or Physical Vapor Deposition (PVD) carbide on the surface of the welded bipolar plate for surface modification. The method has the defects of poor surface modification quality of the welding part and easy corrosion. And the two bipolar plate surface modification methods have the defects of high cost and short service life.
The electrostatic spraying technology is mostly applied to spraying chargeable materials on the surface of a metal conductor, and plastics are hardly used as sprayed hanging parts due to the insulating characteristic of the plastics. When insulating substances are involved in the spraying raw materials, the insulating substances are made to conduct electricity by mixing a certain proportion of conducting solution into the materials; the bipolar plate has low conductivity, and the existing extrusion process cannot further improve the carbon content and reduce the electrode thickness to increase the electric density.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention provides an integrated structure of a bipolar plate and an electrode frame, and a preparation method and application thereof.
The above purpose of the invention is realized by the following technical scheme:
s1, cutting a selected plastic plate into the size of an electrode frame, arranging an electrolyte flow channel or reserving an electrolyte flow channel area at the edge, removing a surface layer in the middle area to form a groove without penetrating the plate, enabling the length and width of the groove to be equal to the size of an electrode, extending the groove to the outermost end with the same depth at one side of the edge without the electrolyte flow channel, and carrying out the same and symmetrical treatment on the two surfaces of the plastic plate, wherein the finished plate is called a substrate;
s2, roughening the bottom of the groove of the substrate prepared in the step S1;
s3, coating a layer of conductive solution on the rough surface of the substrate prepared in the step S2, wherein the conductive solution can enable the surface of the substrate to form a conductive liquid film;
s4, spraying a carbon material coating on the surface of the substrate prepared in the step S3 in an electrostatic spraying manner to prepare an integrated prefabricated plate of the bipolar plate and the electrode frame;
s5, placing the bipolar plate and the electrode frame integrated prefabricated plate manufactured in the step S4 in a vacuum drying box, drying to constant weight, then placing on a hot press for hot pressing, so that the carbon material coating is tightly and firmly combined with the plastic plate, and cooling;
and S6, connecting the carbon material coatings at the extending ports of the grooves on the two sides of the plate by using a conductive material with good conductivity, so as to obtain the bipolar plate and electrode frame integrated structure with high conductivity and strong mechanical property.
Further, in step S1, the plastic plate is made of one of polyethylene, polypropylene, and polyvinylidene fluoride;
further, in the step S3, the conductive solution is a mixed solution of graphite powder and an organic solvent, and the volume percentage is 20: 80;
further, in the step S4, the carbon coating material is a mixture obtained by mixing microcrystalline graphite and conductive carbon black in a mass ratio of 1:1, or carbon 60 with a mass fraction of 2% is added into the mixture;
further, in the step S4, the thickness of the carbon coating material is 0.3-0.5 mm;
further, in step S5, the hot press needs to be preheated in advance, the hot pressing temperature is 155-215 ℃, the hot pressing pressure is 3-5 MPa, and the pressure holding time is more than 3 seconds.
The bipolar plate and electrode frame integrated structure is manufactured by the preparation method and comprises the following steps: a substrate with a groove and extending outwards at one end, a carbon material coating, an electrolyte flow channel and a conductive connecting material; wherein, the groove is internally distributed with carbon material coatings with uniform thickness, the conductive connecting material connects the carbon material coatings at two sides at the extending position of the groove, and the electrolyte flow channels are distributed in the substrate.
Compared with the prior art, the invention has the beneficial effects that:
(1) the applied electrostatic spraying process is opposite to the conventional mode, the plastic plate is subjected to conductive treatment, and the conductive material is sprayed on the surface of the plastic plate, so that the problems that a graphite plate in the bipolar plate of the flow battery is fragile and easy to break and the carbon-plastic composite plate is low in conductivity are solved, the performance advantages of the plastic and the carbon material are fully utilized, and the prepared bipolar plate has excellent mechanical performance and high conductivity;
(2) the bipolar plate and electrode frame integrated structure provided by the invention has a good liquid resistance effect, and can effectively reduce the liquid leakage phenomenon between the bipolar plate and the electrode frame in the operation of the flow battery;
(3) the bipolar plate and electrode frame integrated structure and the preparation method thereof provided by the invention reduce the thickness of the bipolar plate, reserve more space for the design of an electrolyte flow channel in the electrode frame, and can realize the purpose of further reducing the thickness of the electrode and reducing the internal resistance of the electrode.
Drawings
FIG. 1 is a front view of an integrated structure of a bipolar plate and an electrode frame;
fig. 2 is a sectional view of the integrated structure of the bipolar plate and the electrode frame.
In the figure: 1. the structure comprises a substrate, 2, a carbon material coating, 3, a conductive connecting material, 4, an electrolyte flow channel and 5, a groove extending part.
Detailed Description
The invention is described in more detail below with reference to specific examples, without limiting the scope of the invention. Unless otherwise specified, the experimental methods adopted by the invention are all conventional methods, and experimental equipment, materials, reagents and the like used in the experimental method can be obtained from commercial sources.
Example 1
Selecting a polyethylene plate with the thickness of 5.0mm, cutting the polyethylene plate into the size of 200 multiplied by 300mm, arranging an electrolyte flow channel or reserving an electrolyte flow channel area at the edge of 300mm, digging out a groove with the depth of 2.0mm in the middle area, extending the groove to the outermost end of one 200mm edge with the same depth and the width of 50mm, and carrying out the same symmetrical treatment on the two surfaces of the plastic plate, wherein the finished plate is called a substrate; roughening the bottom of the groove of the substrate, and coating a layer of conductive solution formed by mixing 1000-mesh graphite powder and butyl lactate according to the volume ratio of 20:80 on the rough surface of the substrate; spraying a carbon material coating layer with the thickness of 0.3mm on the surface of the substrate by adopting an electrostatic spraying process, wherein the sprayed carbon material is a mixture obtained by mixing microcrystalline graphite and conductive carbon black according to the mass ratio of 1:1, so as to obtain the bipolar plate and electrode frame integrated prefabricated plate; placing the bipolar plate and the electrode frame integrated prefabricated plate in a vacuum drying box, drying to constant weight, then placing on a hydraulic hot press preheated in advance at the temperature of 155 +/-5 ℃ for hot pressing, wherein the hot pressing pressure is 5MPa, and the pressure holding time is 4 seconds, so that the carbon material coating is tightly and firmly combined with the plastic plate, and cooling; and connecting the carbon material coatings at the extending ports of the grooves on the two sides of the plate by using a fastener made of a copper material prepared in advance to obtain the bipolar plate and electrode frame integrated structure with high conductivity and strong mechanical property.
Example 2
The difference between this embodiment and embodiment 1 is that the material of the substrate is selected to be polypropylene, and the conductive solution is formed by mixing 1000 mesh graphite powder and acetone, wherein the volume ratio of the graphite powder to the acetone is 20: 80.
Example 3
The difference between this embodiment and embodiment 1 is that the material of the substrate is selected to be polypropylene, and the conductive solution is formed by mixing 1000 mesh graphite powder and acetone, wherein the volume ratio of the graphite powder to the acetone is 10: 90.
Example 4
The difference between this embodiment and embodiment 1 is that the material of the substrate is selected to be polypropylene, and the conductive solution is formed by mixing 1000 mesh graphite powder and acetone, wherein the volume ratio of the graphite powder to the acetone is 30: 70.
Example 5
Selecting a polyvinylidene fluoride plate with the thickness of 5.0mm, cutting the polyvinylidene fluoride plate into the size of 200 multiplied by 300mm, arranging an electrolyte flow channel or reserving an electrolyte flow channel area at the edge of 300mm, digging out a groove with the depth of 2.0mm in the middle area, extending the groove to the outermost end of one 200mm edge with the same depth and the width of 50mm, carrying out the same symmetrical treatment on the two surfaces of the plastic plate, and calling the finished plate as a substrate; roughening the bottom of the groove of the substrate, and coating a layer of conductive solution formed by mixing 1000-mesh graphite powder and cyclohexanone according to a volume ratio of 20:80 on the rough surface of the substrate; spraying a carbon material coating layer with the thickness of 0.3mm on the surface of the substrate by adopting an electrostatic spraying process, wherein the sprayed carbon material is a mixture obtained by mixing microcrystalline graphite and conductive carbon black according to the mass ratio of 1:1, so as to obtain the bipolar plate and electrode frame integrated prefabricated plate; placing the bipolar plate and the electrode frame integrated prefabricated plate in a vacuum drying box, drying to constant weight, then placing on a hydraulic hot press preheated in advance at the temperature of 215 +/-5 ℃ for hot pressing, wherein the hot pressing pressure is 3MPa, the pressure holding time is 3 seconds, so that the carbon material coating is tightly and firmly combined with the plastic plate, and cooling; the carbon material coatings at the groove extending ports on the two sides of the plate are connected by a fastener made of copper material prepared in advance, and the bipolar plate and electrode frame integrated structure with high conductivity and strong mechanical property is obtained.
Example 6
This example is different from example 5 in that the thickness of the carbon material electrostatically sprayed on the substrate surface was 0.1 mm.
Example 7
This example is different from example 5 in that the thickness of the carbon material electrostatically sprayed on the substrate surface was 0.5 mm.
Example 8
This example is different from example 5 in that the thickness of the carbon material electrostatically sprayed on the substrate surface was 0.6 mm.
Example 9
This example differs from example 5 in that the carbon material electrostatically sprayed on the substrate surface had a thickness of 0.5mm, and 2 mass% of carbon 60 was added to the carbon material sprayed blend.
Example 10
The present embodiment is different from embodiment 5 in that the depth of the groove is formed to be greater than 2.0mm, so that the remaining thickness at the groove of the substrate is less than 1.0 mm.
The phenomena observed in the processing processes of the embodiments 1 to 10 of the invention are compared, and the conductivity of the carbon material coating layer of the bipolar plate and electrode frame integrated structure of the final product is tested, and the related results are shown in table 1.
TABLE 1 test data and associated description for samples prepared in examples 1-10
The test data and the process phenomenon description of the embodiment show that the method provided by the invention can be used for preparing the bipolar plate and electrode frame integrated structure made of various types of plastic materials according to a specific environment, and the integrated structure can simultaneously have stronger mechanical property and corrosion resistance of a plastic substrate and higher electrical conductivity of a carbon material; in the aspect of the preparation proportion of the conductive solution, too much graphite powder can cause the carbon material coating and the substrate to be combined firmly in the electrostatic spraying process, gaps exist, too little graphite powder can cause the surface of the substrate to have poor conductivity, too much raw materials are wasted in the initial stage of spraying, and the volume percentage of the graphite powder mixed with the solvent is about 20-80, so that a better effect can be obtained; from the analysis of the examples given in the present invention, 0.5mm is a relatively ideal choice, and the conductivity of the carbon material coating is further improved by adding some carbon-containing excellent conductive material (such as carbon 60) during the electrostatic spraying process.
Example 11
The bipolar plate obtained in example 7 and the electrode frame integrated structure were assembled into a 10kw stack for experiments, and compared with the 10kw stack assembled with the PP carbon plastic composite bipolar plate produced by the extrusion process in the institute of chemical and physical research in the same operation mode, and the average voltage efficiency value of the first 30 cycles was taken as the evaluation result. Specifically, as shown in table 2.
TABLE 2 evaluation results of the voltage efficiency of the cell stack
It is known that the electrical conductivity of the bipolar plate is a key factor affecting the voltage efficiency of the stack, and particularly, the high-conductivity bipolar plate has a significant effect on the voltage efficiency compared with the bipolar plate with lower electrical conductivity. The voltage efficiency of the bipolar plate manufactured by the invention is improved by more than 2 percent compared with that of a PP carbon plastic composite plate.
The embodiments described above are merely preferred embodiments of the invention, rather than all possible embodiments of the invention. Any obvious modifications to the above would be obvious to those of ordinary skill in the art, but would not bring the invention so modified beyond the spirit and scope of the present invention.
Claims (9)
1. A preparation method of a bipolar plate and electrode frame integrated structure is characterized by comprising the following steps:
s1, selecting a plastic plate to be cut into the size of an electrode frame, arranging an electrolyte flow channel or reserving an electrolyte flow channel area at the edge, scratching the surface layer in the middle area to form a groove without penetrating the plate, enabling the length and width of the groove to be equal to the size of the electrode, then enabling the groove to extend to the outermost end with the same depth at one side of the edge without the electrolyte flow channel, and carrying out the same and symmetrical treatment on the two surfaces of the plastic plate, so that the finished plate is called a substrate;
s2, roughening the bottom of the groove of the substrate prepared in the step S1;
s3, coating a layer of conductive solution on the rough surface of the substrate prepared in the step S2, wherein the conductive solution can enable the surface of the substrate to form a conductive liquid film;
s4, spraying a carbon material coating on the surface of the substrate prepared in the step S3 in an electrostatic spraying manner to prepare an integrated prefabricated plate of the bipolar plate and the electrode frame;
s5, placing the bipolar plate and the electrode frame integrated prefabricated plate manufactured in the step S4 in a vacuum drying box, drying to constant weight, then placing on a hot press for hot pressing, so that the carbon material coating is tightly and firmly combined with the plastic plate, and cooling;
and S6, connecting the carbon material coatings at the extending ports of the grooves on the two sides of the plate by using a conductive material with good conductivity, so as to obtain the bipolar plate and electrode frame integrated structure with high conductivity and strong mechanical property.
2. The method as claimed in claim 1, wherein the plastic sheet is selected from the group consisting of polyethylene, polypropylene, and polyvinylidene fluoride in step S1.
3. The method of claim 1, wherein the conductive solution in step S3 is a mixed solution of graphite powder and organic solvent, and the volume percentage is 20: 80.
4. The method of claim 1, wherein the carbon coating material in step S4 is a mixture of microcrystalline graphite and conductive carbon black in a mass ratio of 1:1, or the mixture is added with 2% by mass of carbon 60.
5. The method of claim 1, wherein the thickness of the carbon coating material in step S4 is 0.3-0.5 mm.
6. The method of claim 1, wherein the hot press machine in step S5 is preheated in advance at a hot pressing temperature of 155-215 ℃, a hot pressing pressure of 3-5 MPa, and a pressure holding time of 3 seconds or more.
7. A bipolar plate and electrode frame integrated structure as claimed in claim 1, which is manufactured by the above manufacturing method, comprising: a substrate (1) with a groove and extending outwards at one end, a carbon material coating (2), an electrolyte flow channel (4) and a conductive connecting material (3); wherein, the carbon material coatings (2) with uniform thickness are distributed in the grooves, the conductive connecting materials (3) connect the carbon material coatings (2) at two sides at the extending positions (5) of the grooves, and the electrolyte runners (4) are distributed in the substrate (1).
8. A preparation method of a bipolar plate and electrode frame integrated structure is applied to a flow battery.
9. An application of a bipolar plate and electrode frame integrated structure in a flow battery.
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| Application Number | Priority Date | Filing Date | Title |
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| CN2020116367092 | 2020-12-31 | ||
| CN202011636709 | 2020-12-31 |
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| CN112786911A true CN112786911A (en) | 2021-05-11 |
| CN112786911B CN112786911B (en) | 2022-02-11 |
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Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101651220A (en) * | 2009-07-15 | 2010-02-17 | 中南大学 | High-tightness flow battery |
| CN102244212A (en) * | 2011-05-25 | 2011-11-16 | 深圳市金钒能源科技有限公司 | Sealing method for galvanic pile of vanadium liquid flow battery and galvanic pile unit and galvanic pile of vanadium liquid flow battery |
| CN107293766A (en) * | 2017-06-27 | 2017-10-24 | 上海中弗新能源科技有限公司 | A kind of integrated bipolar plates for SOFC |
| CN108470931A (en) * | 2018-03-15 | 2018-08-31 | 大连交通大学 | A kind of fuel cell metal double polar plates surface corrosion-resistant erosion method of modifying |
| CN110620240A (en) * | 2018-06-19 | 2019-12-27 | 北京普能世纪科技有限公司 | Preparation method of integrated electrode and vanadium redox flow battery |
| CN111326758A (en) * | 2018-11-28 | 2020-06-23 | 中国科学院大连化学物理研究所 | Zinc-bromine single flow battery |
-
2021
- 2021-01-18 CN CN202110063172.3A patent/CN112786911B/en active Active
Patent Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101651220A (en) * | 2009-07-15 | 2010-02-17 | 中南大学 | High-tightness flow battery |
| CN102244212A (en) * | 2011-05-25 | 2011-11-16 | 深圳市金钒能源科技有限公司 | Sealing method for galvanic pile of vanadium liquid flow battery and galvanic pile unit and galvanic pile of vanadium liquid flow battery |
| CN107293766A (en) * | 2017-06-27 | 2017-10-24 | 上海中弗新能源科技有限公司 | A kind of integrated bipolar plates for SOFC |
| CN108470931A (en) * | 2018-03-15 | 2018-08-31 | 大连交通大学 | A kind of fuel cell metal double polar plates surface corrosion-resistant erosion method of modifying |
| CN110620240A (en) * | 2018-06-19 | 2019-12-27 | 北京普能世纪科技有限公司 | Preparation method of integrated electrode and vanadium redox flow battery |
| CN111326758A (en) * | 2018-11-28 | 2020-06-23 | 中国科学院大连化学物理研究所 | Zinc-bromine single flow battery |
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