CN108832153B - Flow field plate of proton exchange membrane fuel cell - Google Patents
Flow field plate of proton exchange membrane fuel cell Download PDFInfo
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- CN108832153B CN108832153B CN201810666630.0A CN201810666630A CN108832153B CN 108832153 B CN108832153 B CN 108832153B CN 201810666630 A CN201810666630 A CN 201810666630A CN 108832153 B CN108832153 B CN 108832153B
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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
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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
- H01M8/0206—Metals or alloys
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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
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- 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 discloses a flow field plate of a proton exchange membrane battery, which comprises a metal substrate and a coating arranged on the metal substrate; the metal substrate is an aluminum flow field plate with the thickness, and the coating comprises an anti-corrosion coating, a polyacetylene layer and a graphene metal composite film; the thickness of the aluminum flow field plate is 100-; the anticorrosive coating is a compact graphene coating formed on the surface of the aluminum flow field plate; the polyacetylene layer and the graphene metal composite film are alternately and repeatedly arranged on the outer side of the anti-corrosion coating, and the repetition frequency is 3-8 times. The problem of corrosion of the aluminum flow field plate in the fuel cell environment is solved.
Description
Technical Field
The invention relates to a flow field plate of a proton exchange membrane fuel cell.
Background
A fuel cell is a power generation device that can directly convert fuel and oxidant into electric energy through an electrode reaction with high efficiency. Proton Exchange Membrane Fuel Cells (PEMFC) are fuel cells in which a solid Proton exchange membrane is used as an electrolyte, hydrogen or methanol is used as a fuel, and air or oxygen is used as an oxidant.
The core of the PEMFC is the MEA (membrane electrode assembly), which is the site of electrochemical reaction, and the dual-flow field plate, which achieves uniform gas distribution, current collection, and water drainage. For gas distribution and current collection, dual flow field plates are generally required to have good electrical conductivity, thermal conductivity, resistance to penetration by fuels and oxidants, and corrosion resistance in an electrochemical environment. The dual-flow field plate comprises two flow field plates which are matched, the flow field plates are various, common porous flow fields and mesh flow field plates constructed by various metal meshes, punctiform flow field plates, partial snake-shaped flow field plates, interdigital flow field plates and the like are provided.
In the prior art, a conductive and corrosion-resistant coating is usually coated on the surface of a metal flow field plate, the commonly used metal flow field plate is stainless steel, and compared with aluminum alloy, the stainless steel and the aluminum alloy have the same price, but the stainless steel has a complex preparation process, the aluminum alloy has a simple preparation process, but the aluminum has active and unstable chemical properties, and how to apply the aluminum alloy to the flow field plate is a technical problem which needs to be solved urgently by a person skilled in the art.
Disclosure of Invention
The invention provides a flow field plate of a proton exchange membrane fuel cell, which solves the corrosion problem of an aluminum flow field plate in a fuel cell environment.
The technical scheme of the invention is realized as follows:
a flow field plate of proton exchange membrane fuel cell comprises a metal substrate and a coating arranged on the metal substrate; the metal substrate is an aluminum flow field plate with the thickness, and the coating comprises an anti-corrosion coating, a polyacetylene layer and a graphene metal composite film; the thickness of the aluminum flow field plate is 100-; the anticorrosive coating is a compact graphene coating formed on the surface of the aluminum flow field plate; the polyacetylene layer and the graphene metal composite film are alternately and repeatedly arranged on the outer side of the anticorrosive coating, and the repetition frequency is 3-8 times;
wherein the pretreated aluminum flow field plate is put into 0.05-5mg/ml graphene oxide aqueous solution containing tetrahydroxy aluminate ions with the concentration of 1-100mmol/L for soaking for 2-24 hours, and the soaking temperature is 20-100 ℃; taking out, drying, and treating in 20-160g/L sodium hypophosphite solution at 20-100 deg.C for 2-24 hr; taking out, cleaning and drying to form a compact graphene coating on the surface of the aluminum flow field plate;
putting the aluminum flow field plate into an acetone solution, adopting a three-electrode system, introducing acetylene gas into the aluminum flow field plate serving as a working electrode, wherein the current low potential is-1.5V, the current density is 30mA/cm2, and the polarization time is 150-220s, and forming a polyacetylene layer on the aluminum flow field plate;
the graphene metal composite membrane is in an ordered and compact graphene laminated structure, covalent bonds exist between the graphene membrane and the membrane, a large number of spherical or hemispherical metal fine particles exist at the edge and the defect, the particle diameter is between 5 and 300nm, and the number ratio of metal element yards to carbon atoms is 0.5 to 10 percent.
Optionally, the concentration of the tetrahydroxy aluminate ions is 3-80 mmol/L; the concentration of the graphene oxide aqueous solution is 0.1-3 mg/mL; the dipping temperature of the aluminum flow field plate in the solution is 30-90 ℃, and the dipping time is 3-18 hours.
Optionally, the concentration of the sodium hypophosphite solution is 30-120 g/L; the treatment temperature of the aluminum flow field plate in the solution is 40-180 ℃, and the treatment time is 4-18 hours.
Optionally, the metal in the graphene metal composite film is copper, nickel, manganese, zinc, or silver.
Optionally, adding a metal ion aqueous solution with a predetermined concentration into the single-layer graphene oxide solution, respectively making an anode and a cathode with the aluminum flow field plate with the polyacetylene layer and the platinum sheet, increasing the voltage by 20V with a direct-current stabilized voltage supply, performing electrophoresis for 1min, forming a layer of film on the aluminum flow field plate at the anode, and performing dehydration and drying at 40 ℃ in a vacuum box to obtain an electrochemically deposited graphene oxide film; and then placing the aluminum flow field plate into a tubular quartz furnace for high-temperature hydrogen-oxygen reduction so as to embed the metal fine particles into the graphene composite membrane.
Optionally, the thickness of the coating is 180-210 nm.
By adopting the technical scheme, the invention has the beneficial effects that:
an anticorrosive coating is arranged on the surface of the aluminum flow field plate, tetrahydroxy aluminate ions with certain concentration are introduced into a graphene oxide aqueous solution, and a layer of compact graphene is coated on the surface of the aluminum flow field plate by a chemical impregnation method and related technical means. The chloride ions generated in the dipping process enable the graphene oxide and the aluminum flow field plate to be crosslinked, the bonding force of the coating is enhanced, and the aluminum ions are continuously generated to enable the graphene oxide layer to be stacked, so that the graphene oxide flow field plate is very compact. Although the graphene oxide layer is very dense, the polyacetylene layer and the graphene metal composite film are alternately and repeatedly arranged outside the graphene oxide layer due to the porosity of the graphene oxide layer. The thickness of the polyacetylene layer is 12-22nm, in the graphene metal composite film, metal fine particles are embedded into the composite film, gaps of graphene can be plugged, the polyacetylene layer and the graphene metal composite film are shielded, and the corrosion resistance of the coating is further improved.
Drawings
In order to more clearly explain the technical solution of the present application, the drawings needed to be used in the embodiments will be briefly described below, and it is obvious to those skilled in the art that other drawings can be obtained according to the drawings without any creative effort.
Fig. 1 is a schematic structural diagram of an embodiment of a flow field plate of a pem fuel cell provided in the present application.
Wherein: 1. metal substrate 2, anticorrosive coating 3, polyacetylene layer 4, graphite alkene metal complex film.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The invention provides a flow field plate of a proton exchange membrane fuel cell, which comprises a metal substrate 1 and a coating arranged on the metal substrate 1; the metal substrate 1 is an aluminum flow field plate with the thickness, and the coating comprises an anticorrosive coating 2, a polyacetylene layer 2 and a graphene metal composite film 4; the thickness of the aluminum flow field plate is 100-; the anticorrosion coating 2 is a compact graphene coating formed on the surface of the aluminum flow field plate; the polyacetylene layer 3 and the graphene metal composite film 4 are alternately and repeatedly arranged on the outer side of the anticorrosive coating 2, and the repetition frequency is 3-8 times;
wherein the pretreated aluminum flow field plate is put into 0.05-5mg/ml graphene oxide aqueous solution containing tetrahydroxy aluminate ions with the concentration of 1-100mmol/L for soaking for 2-24 hours, and the soaking temperature is 20-100 ℃; taking out, drying, and treating in 20-160g/L sodium hypophosphite solution at 20-100 deg.C for 2-24 hr; taking out, cleaning and drying to form a compact graphene coating on the surface of the aluminum flow field plate;
putting the aluminum flow field plate into an acetone solution, adopting a three-electrode system, introducing acetylene gas into the aluminum flow field plate serving as a working electrode, wherein the current low potential is-1.5V, the current density is 30mA/cm2, and the polarization time is 150-220s, and forming a polyacetylene layer 3 on the aluminum flow field plate;
the graphene metal composite film 4 is in an ordered and compact graphene laminated structure, covalent bonds exist between graphene films, a large number of spherical or hemispherical metal fine particles exist at edges and defects, the particle diameter is between 5 and 300nm, and the ratio of the number of metal element yards to the number of carbon atoms is 0.5 to 10%.
An anticorrosive coating 2 is arranged on the surface of the aluminum flow field plate, tetrahydroxy aluminate ions with certain concentration are introduced into a graphene oxide aqueous solution, and a layer of compact graphene is coated on the surface of the aluminum flow field plate by using a chemical impregnation method and related technical means. The chloride ions generated in the dipping process enable the graphene oxide and the aluminum flow field plate to be crosslinked, the bonding force of the coating is enhanced, and the aluminum ions are continuously generated to enable the graphene oxide layer to be stacked, so that the graphene oxide flow field plate is very compact. Although the graphene oxide layer is very dense, the polyacetylene layer 3 and the graphene metal composite film 4 are alternately and repeatedly disposed outside the graphene oxide layer due to the porosity of the graphene oxide layer. The thickness of the polyacetylene layer 3 is 12-22nm, in the graphene metal composite film 4, metal fine particles are embedded into the composite film, gaps of graphene can be plugged, the polyacetylene layer and the graphene metal composite film are shielded, and the corrosion resistance of the coating is further improved.
Specifically, the concentration of the tetrahydroxy aluminate ions is 3-80 mmol/L; the concentration of the graphene oxide aqueous solution is 0.1-3 mg/mL; the dipping temperature of the aluminum flow field plate in the solution is 30-90 ℃, and the dipping time is 3-18 hours.
The concentration of the sodium hypophosphite solution is 30-120 g/L; the treatment temperature of the aluminum flow field plate in the solution is 40-180 ℃, and the treatment time is 4-18 hours.
The process has the advantages of simple coating method, convenient operation, lower cost, high operation efficiency and lower requirements on technical personnel compared with methods such as electroplating, chemical plating, physical vapor deposition and the like.
In each of the above specific embodiments, the metal in the graphene metal composite film is copper, nickel, manganese, zinc, or silver.
Further, adding a metal ion aqueous solution with a preset concentration into the single-layer graphene oxide solution, respectively using the aluminum flow field plate with the polyacetylene layer and the platinum sheet as an anode and a cathode, increasing the voltage by 20V by using a direct-current stabilized voltage supply, performing electrophoresis for 1min, forming a layer of film on the aluminum flow field plate at the anode, and performing dehydration and drying at 40 ℃ in a vacuum box to obtain an electrochemical deposition graphene oxide film; and then placing the aluminum flow field plate into a tubular quartz furnace for high-temperature hydrogen-oxygen reduction so as to embed the metal fine particles into the graphene composite membrane.
Specifically, the thickness of the coating is 180-210 nm.
The metal ions support the graphene film, form metal particles and are embedded into the graphene powder film, so that gaps of graphene are filled, and the conductivity of the graphene film is further enhanced. The mode can prepare composite films of various metals and graphene, the whole process is convenient to operate, and the adjustable degree is high.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents, improvements and the like that fall within the spirit and principle of the present invention are intended to be included therein.
Claims (4)
1. A flow field plate of a proton exchange membrane fuel cell is characterized by comprising a metal substrate and a coating arranged on the metal substrate; the metal substrate is an aluminum flow field plate, and the coating comprises an anticorrosive coating, a polyacetylene layer and a graphene metal composite film; the metal in the graphene metal composite film is copper, nickel, manganese, zinc and silver; the thickness of the aluminum flow field plate is 100-; the anticorrosive coating is a compact graphene coating formed on the surface of the aluminum flow field plate; the polyacetylene layer and the graphene metal composite film are alternately and repeatedly arranged on the outer side of the anticorrosive coating, and the repetition frequency is 3-8 times;
wherein, the aluminum flow field plate is put into 0.05-5mg/ml graphene oxide aqueous solution containing tetrahydroxy aluminate ions with the concentration of 1-100mmol/L for dipping for 2-24 hours, and the dipping temperature is 20-100 ℃; taking out, drying, and treating in 20-160g/L sodium hypophosphite solution at 20-100 deg.C for 2-24 hr; taking out, cleaning and drying to form a compact graphene coating on the surface of the aluminum flow field plate;
placing the aluminum flow field plate with the compact graphene coating in an acetone solution, adopting a three-electrode system, taking the aluminum flow field plate with the compact graphene coating as a working electrode, introducing acetylene gas, wherein the current has a low potential of-1.5V and a current density of 30mA/cm2The polarization time is 150-;
adding a metal ion aqueous solution with a preset concentration into a single-layer graphene oxide solution, respectively taking an aluminum flow field plate with a compact graphene coating layer and a platinum sheet with a polyacetylene layer as an anode and a cathode, increasing the voltage by 20V by using a direct-current stabilized voltage supply, performing electrophoresis for 1min, forming a layer of film on the aluminum flow field plate with the compact graphene coating layer and the polyacetylene layer at the anode, and performing dehydration and drying at 40 ℃ in a vacuum box to obtain an electrochemical deposition graphene oxide film; then placing the aluminum flow field plate with the polyacetylene layer, the compact graphene coating and the electrochemically deposited graphene oxide film into a tubular quartz furnace for high-temperature hydrogen-oxygen reduction so as to embed metal fine particles into the graphene composite film;
the graphene metal composite membrane is in an ordered and compact graphene laminated structure, covalent bonds exist between the graphene membrane and the membrane, a large number of spherical or hemispherical metal fine particles exist at the edge and the defect, the particle diameter is between 5 and 300nm, and the number ratio of metal element yards to carbon atoms is 0.5 to 10 percent.
2. A flow field plate for a proton exchange membrane fuel cell according to claim 1, wherein the concentration of the tetrahydroxy aluminate ions is 3 to 80 mmol/L; the concentration of the graphene oxide aqueous solution is 0.1-3 mg/mL; the dipping temperature of the aluminum flow field plate in the solution is 30-90 ℃, and the dipping time is 3-18 hours.
3. A flow field plate for a pem fuel cell according to claim 1 wherein said sodium hypophosphite solution has a concentration of 30-120 g/L; the treatment temperature of the aluminum flow field plate in the solution is 40-180 ℃, and the treatment time is 4-18 hours.
4. A flow field plate for a pem fuel cell according to claim 1 wherein said coating has a thickness of 180-210 nm.
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