CN114361493B - Plastic fuel cell system - Google Patents
Plastic fuel cell system Download PDFInfo
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- CN114361493B CN114361493B CN202111429007.1A CN202111429007A CN114361493B CN 114361493 B CN114361493 B CN 114361493B CN 202111429007 A CN202111429007 A CN 202111429007A CN 114361493 B CN114361493 B CN 114361493B
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- 239000004033 plastic Substances 0.000 title claims abstract description 117
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Classifications
-
- 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
Landscapes
- Inert Electrodes (AREA)
Abstract
The invention discloses a plastic fuel cell system, and belongs to the technical field of fuel cell materials. The invention combines plastic, carbon-based electrocatalyst and conductive agent to form a composite material cathode, and the composite material cathode is directly used in a fuel cell system. In the liquid electrolyte with a stable electrochemical window, the carbon-based catalyst is utilized to reduce the electrochemical oxidation reaction energy barrier of the plastic, so that the complete oxidation process of the plastic is realized, and stable voltage and current output is obtained. The invention has simple operation, is suitable for various plastic materials, provides a wide prospect for recycling waste plastic products, and does not provide a new way for acquiring novel clean energy.
Description
Technical field:
The invention relates to the technical field of fuel cells, in particular to a plastic fuel cell system.
The background technology is as follows:
The total amount of plastic products such as polyethylene, polyethylene terephthalate, polyamide and the like which are produced in a cumulative way worldwide at present reaches 80 hundred million tons, wherein only 9 percent of the plastic products are recycled, 12 percent of the plastic products are degraded by incineration, and the rest 79 percent of the waste plastic products can only be treated by land or deep sea landfill. The buried waste plastic products are difficult to degrade naturally even after hundreds of years, and can bring great harm to the natural environment. The only method capable of rapidly eliminating the pollution of waste plastics at present is to deconstruct the plastics by heat treatment, for example, elements such as C, H, O, N in the plastics are directly converted into gases such as CO 2、H2O、NO2 by combustion or the plastics are converted into monomers by pyrolysis. The above method has the disadvantage that the plastics are difficult to burn sufficiently in air with the concomitant generation of a large amount of toxic, harmful gases. The treatment of plastics by means of pyrolysis leads to a considerable energy consumption. Therefore, the development of a controllable, green, environment-friendly, low-energy-consumption and even energy-consumption-free method for degrading and converting waste plastics has great significance for relieving the environmental hazard brought by plastic products.
In order to solve the problems, the plastic fuel cell system is utilized to degrade and convert the plastic in an electrochemical mode, so that pollution-free degradation of the plastic can be realized, and chemical energy can be directly converted into electric energy to be used as clean energy. Therefore, the process can realize the reutilization of the carbon-containing waste and generate clean energy, and has great significance for realizing the targets of carbon peak reaching and carbon neutralization.
The invention comprises the following steps:
In order to realize recycling of waste plastic products, the invention aims to provide a plastic fuel cell system. Through reasonable design and selection of electrolyte, catalyst, current collector, binder, conductive agent and diaphragm, and preparation of plastic composite negative electrode, the plastic composite negative electrode can realize effective electrochemical complete oxidative degradation of waste plastic after matching with oxygen or air positive electrode, and output electric energy as clean energy.
In order to achieve the above purpose, the technical scheme adopted by the invention is as follows:
A plastic fuel cell system comprising a plastic composite anode, a separator, an oxygen or air porous anode, and a liquid electrolyte, wherein: the plastic composite anode takes plastic as anode active material, and anode slurry containing plastic, anode catalyst, conductive agent and binder is coated on an anode current collector and dried to prepare the plastic composite anode; the oxygen or air porous anode is a porous sheet structure formed by pressing and compounding a negative electrode membrane containing an anode catalyst and a conductive agent with an anode current collector with meshes; and placing the plastic composite negative electrode, the isolating film, the oxygen or air positive electrode and the electrolyte in a shell of the button cell or the electrolytic cell, placing the obtained integral structure in an oxygen-containing atmosphere, and then utilizing an electrochemical workstation to connect current collectors of the positive electrode and the negative electrode to monitor the discharge voltage and the current of the battery system.
The plastic is polyethylene, polypropylene, polyvinyl chloride, polystyrene, polytetrafluoroethylene, polymethyl methacrylate, polyethylene terephthalate, polyether ether ketone and other plastics containing carbon, hydrogen, oxygen, sulfur, nitrogen, fluorine and other elements or chemical modified derivatives thereof.
The negative electrode catalyst is a carbon-based catalyst, and the carbon-based catalyst is a metal and/or nonmetal element doped modified carbon material (one or more of graphene, carbon nano tube, graphite alkyne, porous carbon, graphite and carbon black); or the carbon-based catalyst is a composite of a metal and/or nonmetal element doped modified carbon material and an inorganic nonmetal material, an organic material or a metal material.
The liquid electrolyte is prepared by dissolving electrolyte in a solvent, and the concentration of the electrolyte is 0-20mol/L; the solvent is one or more of water, ethers, esters, ketones, aldehydes and ionic liquid, and the electrolyte is one or more of monobasic or polybasic organic acid, inorganic acid, alkali and salt.
In the plastic fuel cell system, a part of the cell shell corresponding to the upper part of the oxygen or air porous anode is of a porous structure; the oxygen-containing atmosphere (the gas used by the anode) is pure oxygen or air, or the oxygen-containing atmosphere is various mixed gases containing oxygen components in any proportion.
The positive electrode catalyst is made of various pure metals such as metal foil, iron, copper and the like; or the positive electrode catalyst is various nonmetallic materials such as boron nitride, copper oxide or nickel phosphide; or the positive electrode catalyst is a composite of one or more of various carbon materials such as graphene, carbon nano tubes and the like and modified materials thereof.
The negative electrode current collector and the positive electrode current collector are made of conductive copper, aluminum, iron or nickel and the like; or the materials of the negative electrode current collector and the positive electrode current collector are alloys (such as copper-zinc alloy and the like); or the materials of the negative electrode current collector and the positive electrode current collector are conductive carbon materials.
The binder is one of sodium carboxymethyl cellulose, lithium carboxymethyl cellulose, styrene-butadiene rubber, polyvinylidene fluoride and polytetrafluoroethylene; the conductive agent is one powder material of carbon nano tube, carbon black, ketjen black and graphene.
The isolating film is one or more of polyethylene, polypropylene, proton exchange film, anion exchange film, glass fiber, cellulose and other insulating materials.
The plastic composite negative electrode is prepared by the following two modes:
The first mode is a hot melt method, and the preparation process is as follows: firstly, uniformly mixing the plastics, the negative electrode catalyst and the conductive agent through mechanical ball milling, wherein the mass fraction of the plastics in the obtained mixed material is 1-99%; then placing the mixed material into an oven, heating to a temperature above the glass transition temperature of the plastic (100-300 ℃) and standing for 2-24 hours; and then uniformly mixing the obtained product with a binder and a conductive agent, preparing negative electrode slurry by using an organic solvent (N-methyl-2-pyrrolidone and the like) or water, then scraping the negative electrode slurry onto the surface of a negative electrode current collector, wherein the scraping thickness is 1-50 mu m, and drying to obtain the plastic composite negative electrode.
The second mode is a solution evaporation method, and the preparation process is as follows: firstly, uniformly mixing the plastic, the negative electrode catalyst, the binder and the conductive agent, wherein the mass fraction of the plastic in the obtained mixed material is 1-99%; and then mixing the mixed material with an organic solvent (one or more of toluene, xylene, N-dimethylformamide and the like) to prepare negative electrode slurry, then scraping the negative electrode slurry onto the surface of a negative electrode current collector, wherein the scraping thickness is 1-50 mu m, and drying to obtain the plastic composite negative electrode.
The invention has the advantages and beneficial effects that:
1. the invention provides a novel plastic fuel cell system design.
2. The catalyst of the plastic composite anode can effectively catalyze the rupture of chemical bonds in the plastic in the discharging process, realize the complete oxidation of the plastic in the composite anode in the discharging process and release electric energy.
3. The invention can effectively recycle waste plastic products, has environmental protection value, can convert waste plastic into clean energy for use, has economic value, and meets the overall targets of carbon peak and carbon neutralization.
Description of the drawings:
Fig. 1 is a schematic diagram of a novel plastic fuel cell system according to the present invention.
Fig. 2 is a scanning electron microscope photograph of a plastic composite negative electrode prepared by a melting method.
Fig. 3 is a scanning electron microscope photograph of a plastic composite anode prepared by a direct knife coating method.
Fig. 4 is a scanning electron microscope photograph of the catalyst in the plastic composite anode.
Fig. 5 is a linear voltammogram of the novel plastic fuel cell system of the present invention.
Fig. 6 is a constant current discharge curve of the novel plastic fuel cell system of the present invention.
The specific embodiment is as follows:
The present invention will be described in further detail with reference to specific examples for better understanding of the technical scheme of the present invention by those skilled in the art.
The invention provides a plastic fuel cell system, which comprises a carbon-based electrocatalyst design, a plastic-based composite anode preparation and an electrochemically stable electrolyte design. The plastic fuel cell is obtained by matching a plastic composite negative electrode, an electrolyte and an oxygen or air positive electrode, and electric energy is released by utilizing the electrocatalytic oxidation process of the plastic and is used as clean energy for storage and utilization.
Example 1:
Fig. 1 is a schematic structural diagram of the novel plastic fuel cell system, taking button cells as an example. Firstly, cutting a plastic composite negative electrode coated on the surface of a copper foil current collector into a circular sheet with the diameter of 12mm, placing the circular sheet into a stainless steel negative electrode shell, and sequentially placing a separation film with the diameter of 20mm and a porous positive electrode sheet with the diameter of 15mm above the circular sheet. Adding 30-100 mu L of electrolyte, placing a porous positive electrode battery shell, and finally tightly connecting the positive electrode battery shell and the negative electrode battery shell by using 2-4 screws. The discharge can be performed after the connection of an external circuit in air or in an argon/oxygen mixed atmosphere. After the plastic reactant in the battery is completely oxidized, the battery can be disassembled, and the discharge is continued after a new plastic composite negative electrode is replaced.
Example 2
And preparing the plastic composite negative electrode by a melting method. The method is mainly aimed at plastics with a low melting point and which are not easily dissolved by organic reagents. Polyethylene plastic is taken as an example of the reactive material. First, 100mg of 300-mesh polyethylene plastic particles were weighed, and 80mg of catalyst and 20mg of conductive carbon black were mixed. Grinding with a ball mill at 1000rpm for 15min, and mixing thoroughly. The mixture was then placed in a 20mL hydrothermal kettle and heated at 200deg.C for 12 h. After the treatment, the material was taken out of the hydrothermal kettle, 90mg was weighed and mixed with 10mg of polyvinylidene fluoride binder, 3mL of N-methyl-2-pyrrolidone was added, and the mixture was ground with a ball mill at 1000rpm for 15 minutes to prepare a slurry. And coating the slurry on the surface of a copper foil current collector by using a scraper with the thickness of 20 mu L, and then placing the copper foil current collector in a vacuum oven at 80 ℃ for 12 hours to prepare the plastic composite anode. A scanning electron microscope photograph of the microscopic morphology is shown in FIG. 2.
Example 3
The plastic composite negative electrode is prepared by a direct knife coating method. Example 3 differs from example 2 in that it is more suitable for plastics with a high melting point and a certain solubility in organic agents. Polystyrene is taken as an example. Firstly, 40mg of 300-mesh polystyrene particles, 30mg of catalyst, 20mg of conductive carbon black and 10mg of polyvinylidene fluoride binder are weighed, 3mL of N-methyl-2-pyrrolidone is added, and the mixture is ground for 15min by a ball mill at 1000rpm to prepare slurry. And coating the slurry on the surface of a copper foil current collector by using a scraper with the thickness of 20 mu L, and then placing the copper foil current collector in a vacuum oven at 80 ℃ for 12 hours to prepare the plastic composite anode. A scanning electron microscope photograph of the microscopic morphology is shown in FIG. 3.
Example 4
Example 4 is a method for preparing a catalyst in a plastic composite anode. Taking microporous carbon composite cobalt oxide catalyst as an example. 200mg of microporous carbon was weighed and mixed with 50mL of nitric acid having a concentration of 0.5mol/L and stirred uniformly. The mixture was then placed in a 100mL hydrothermal kettle and hydrothermal treated at 180deg.C for 12h to obtain oxidized microporous carbon. And (3) filtering the solution after the hydrothermal kettle is cooled, cleaning the oxidized microporous carbon with water and ethanol for three times respectively, and then placing the solution in a vacuum oven to dry at 80 ℃ for 12 hours. Weighing 20mg of dried oxidized microporous carbon, adding into 50mL of cobalt chloride solution with the concentration of 1mol/L, mixing and stirring uniformly. And then regulating the pH of the mixed solution to 10 by using ammonia water, and placing the regulated mixed solution into a 100mL hydrothermal kettle, and carrying out hydrothermal reaction at 200 ℃ for 12 hours to prepare the microporous carbon composite cobalt oxide catalyst. A scanning electron microscope photograph of the microscopic morphology is shown in FIG. 4.
Example 5
Example 5 is a porous positive electrode preparation method. 80mg of a commercial platinum/carbon composite catalyst was weighed, 10mg of a conductive agent was uniformly mixed with an aqueous dispersion of polytetrafluoroethylene containing 10mg of polytetrafluoroethylene, and the mixture was ground with a ball mill at 1000rpm for 15 minutes to prepare a slurry. Taking out the slurry, adding a proper amount of ethanol, grinding into soft blocks by using a mortar, and rolling into a membrane with a certain thickness. Cutting the membrane into a disc with the diameter of 15mm, stacking the disc with a stainless steel net current collector with the diameter of 15mm, placing the disc under a hydraulic press, maintaining the pressure for 30s at the pressure of 4Mpa, and then placing the disc in a vacuum oven at the temperature of 60 ℃ for 12h to prepare the porous positive pole piece compounded with the stainless steel current collector.
Example 6
The test method is a full-cell electrochemical performance test of a plastic composite anode matched with an air anode. The button cell is assembled by using a polyethylene terephthalate plastic composite anode added with a microporous carbon composite cobalt oxide catalyst, a porous air anode loaded with a commercial platinum carbon catalyst, a glass fiber diaphragm and a sodium hydroxide aqueous solution electrolyte with the concentration of 2mol/L, and the assembly parameters are shown in an embodiment 1. The button cell was subjected to linear voltammetry scan test using silver/silver chloride as a reference electrode, as shown in fig. 5, the plastic composite negative electrode had a significant oxidation peak at a voltage of 0V (relative to silver/silver chloride), indicating that polyethylene terephthalate plastic was oxidized by the air positive electrode under the action of the porous carbon composite cobalt oxide catalyst. The battery discharge curve is shown in FIG. 6, and the average discharge voltage of the battery was 0.2V and the capacity was 0.6mAh at a current density of 25 mA/g.
The results of the embodiment show that the invention can realize electrochemical oxidation of plastics by reasonably designing the catalyst and the electrolyte, preparing the plastic composite negative electrode and assembling the battery device, and can realize discharge of the battery device by matching with the air positive electrode. The composite anode can be prepared for plastics with different physical and chemical properties by using a melting method or a direct blade coating method. The oxidation process of the polyethylene terephthalate plastic can be realized by adopting the microporous carbon composite cobalt oxide catalyst. The novel plastic fuel cell system has simple design and convenient operation, can realize pollution-free decomposition of waste plastics and generate electric energy as clean energy, provides a new solution for recycling waste plastics and protecting environment, and meets the overall targets of carbon peak and carbon neutralization.
Claims (9)
1. A plastic fuel cell system characterized in that: the plastic fuel cell system comprises a plastic composite anode, a separation membrane, an oxygen or air porous anode and a liquid electrolyte, wherein: the plastic composite anode takes plastic as anode active material, and anode slurry containing plastic, anode catalyst, conductive agent and binder is coated on an anode current collector and dried to prepare the plastic composite anode; the oxygen or air porous anode is a porous sheet structure formed by pressing and compounding a negative electrode membrane containing an anode catalyst and a conductive agent with an anode current collector with meshes; placing the plastic composite negative electrode, the isolating membrane, the oxygen or air positive electrode and the electrolyte in a button cell or an electrolytic cell shell, then placing the obtained integral structure in an oxygen-containing atmosphere, and connecting a current collector of the positive electrode and the negative electrode by using an electrochemical workstation to obtain the plastic fuel cell system; the plastic is polyethylene, polypropylene, polyvinyl chloride, polystyrene, polytetrafluoroethylene, polymethyl methacrylate, polyethylene terephthalate, polyether ether ketone containing carbon, hydrogen, oxygen, sulfur, nitrogen and fluorine or chemical modified derivatives thereof.
2. The plastic fuel cell system according to claim 1, wherein: the negative electrode catalyst is a carbon-based catalyst, the carbon-based catalyst is a carbon material modified by doping metal and/or nonmetal elements, and the carbon material is one or more of graphene, carbon nano tubes, graphite alkyne, porous carbon, graphite and carbon black; or the carbon-based catalyst is a composite of a metal and/or nonmetal element doped modified carbon material and an inorganic nonmetal material, an organic material or a metal material.
3. The plastic fuel cell system according to claim 1, wherein: the liquid electrolyte is prepared by dissolving electrolyte in a solvent, and the concentration of the electrolyte is 0-20 mol/L; the solvent is one or more of water, ethers, esters, ketones, aldehydes and ionic liquid, and the electrolyte is one or more of monobasic or polybasic organic acid, inorganic acid, alkali and salt.
4. The plastic fuel cell system according to claim 1, wherein: in the plastic fuel cell system, a part of the cell shell corresponding to the upper part of the oxygen or air porous anode is of a porous structure; the oxygen-containing atmosphere used by the anode is pure oxygen or air, or the oxygen-containing atmosphere is various mixed gases containing oxygen components in any proportion.
5. The plastic fuel cell system according to claim 1, wherein: the positive electrode catalyst is metal platinum, iron and copper; or the positive electrode catalyst is boron nitride, copper oxide or nickel phosphide; or the positive electrode catalyst is one or a plurality of compounds of graphene, carbon nano tubes and modified materials thereof.
6. The plastic fuel cell system according to claim 1, wherein: the negative electrode current collector and the positive electrode current collector are made of conductive copper, aluminum, iron or nickel; or the materials of the negative electrode current collector and the positive electrode current collector are copper-zinc alloy; or the materials of the negative electrode current collector and the positive electrode current collector are conductive carbon materials.
7. The plastic fuel cell system according to claim 1, wherein: the binder is one of sodium carboxymethyl cellulose, lithium carboxymethyl cellulose, styrene-butadiene rubber, polyvinylidene fluoride and polytetrafluoroethylene; the conductive agent is one powder material of carbon nano tube, carbon black, ketjen black and graphene; the isolating film is one or more of polyethylene, polypropylene, proton exchange film, anion exchange film, glass fiber and cellulose.
8. The plastic fuel cell system according to claim 1, wherein: the plastic composite negative electrode is prepared by adopting a hot melting method, and comprises the following steps: firstly, uniformly mixing the plastic, the negative electrode catalyst and the conductive agent, wherein the mass fraction of the plastic in the obtained mixture is 1-99%; then placing the mixed material into an oven, heating to 100-300 ℃ of plastic glass transition temperature, and standing for 2-24h; and uniformly mixing the obtained product with a binder and a conductive agent, preparing negative electrode slurry by using an N-methyl-2-pyrrolidone organic solvent or water, then scraping the negative electrode slurry onto the surface of a negative electrode current collector, wherein the scraping thickness is 1-50 mu m, and drying to obtain the plastic composite negative electrode.
9. The plastic fuel cell system according to claim 1, wherein: the plastic composite negative electrode is prepared by adopting a solution evaporation method, and comprises the following steps: firstly, uniformly mixing the plastic, the negative electrode catalyst, the binder and the conductive agent, wherein the mass fraction of the plastic in the obtained mixed material is 1-99%; and then mixing the mixed material with an organic solvent, wherein the organic solvent is one or more of toluene, dimethylbenzene and N, N-dimethylformamide, preparing negative electrode slurry, then scraping the negative electrode slurry onto the surface of a negative electrode current collector, and drying to obtain the plastic composite negative electrode, wherein the scraping thickness is 1-50 mu m.
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| CN1901261A (en) * | 2006-07-20 | 2007-01-24 | 复旦大学 | Novel high performance alkaline fuel cell |
| CN101165964A (en) * | 2007-09-20 | 2008-04-23 | 复旦大学 | Asymmetric secondary air fuel battery |
| CN103811688A (en) * | 2012-11-07 | 2014-05-21 | 柯耐克斯系统株式会社 | Solid oxide fuel cell and fuel cell system |
| CN105449186A (en) * | 2015-11-18 | 2016-03-30 | 中国科学院深圳先进技术研究院 | Novel secondary battery and preparation method therefor |
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| CN1901261A (en) * | 2006-07-20 | 2007-01-24 | 复旦大学 | Novel high performance alkaline fuel cell |
| CN101165964A (en) * | 2007-09-20 | 2008-04-23 | 复旦大学 | Asymmetric secondary air fuel battery |
| CN103811688A (en) * | 2012-11-07 | 2014-05-21 | 柯耐克斯系统株式会社 | Solid oxide fuel cell and fuel cell system |
| CN105449186A (en) * | 2015-11-18 | 2016-03-30 | 中国科学院深圳先进技术研究院 | Novel secondary battery and preparation method therefor |
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