CN106935885B - High-porosity porous carbon filled fuel cell flow field structure and preparation method thereof - Google Patents
High-porosity porous carbon filled fuel cell flow field structure and preparation method thereof Download PDFInfo
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- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
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- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
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Abstract
The invention belongs to the field of fuel cell flow field design, and particularly relates to a high-porosity porous carbon filled fuel cell flow field structure and a preparation method thereof. The fuel cell flow field structure is a porous carbon structure with high porosity filled in a flow channel of a fuel cell bipolar plate; wherein the porosity of the porous carbon is 50% -90%. The porous carbon structure with good wettability, high strength and high porosity is prepared by utilizing the gelation stage of the phenolic resin, and the porous carbon is filled in the flow channel of the bipolar plate of the fuel cell so as to enhance the water management capability of the bipolar plate. Compared with the conventional preparation method of the porous carbon structure, the method provided by the invention is quicker, milder in conditions and more flexible in selection of experimental conditions. The method has the advantages of simple equipment, common chemical raw materials for synthesizing the materials, low cost, simple and quick preparation process, mild conditions and suitability for large-scale industrial production.
Description
Technical Field
The invention belongs to the field of fuel cell flow field design, and particularly relates to a high-porosity porous carbon filled fuel cell flow field structure and a preparation method thereof.
Background
The performance of Proton Exchange Membrane Fuel Cells (PEMFCs) is related to the accumulation of water in the cell, and when the amount of water increases with the accompanying degradation of the membrane, the performance of the cell rapidly decreases, thus leading to an imbalance in the state of water in the cell and a decrease in the performance of the cell in the case of poor water management. Ensuring water balance among the various parts of the PEM cell is critical, otherwise the life of the fuel cell will be directly affected.
The method for controlling water balance comprises the following steps: selecting proper membrane materials, optimally designing the membrane electrode and the cell structure, adjusting the inlet air humidity of reaction gas and the like. The electrode structure and the flow field structure are improved, so that the discharge of redundant water in the cell can be facilitated, and the phenomenon of cathode flooding is avoided. In addition, the material and surface of the bipolar plate can be improved to achieve the purpose of storing or distributing water. For example, shelkhin proposes to lay hydrophilic strips on the flow channels on both sides of the bipolar plate, the hydrophilic strips are made of inert hydrophilic materials, such as filter paper and glass fiber, the hydrophilic strips on the cathode side uniformly absorb and store excess water when the cell is in operation, and the water stored in the hydrophilic strips can supply the membrane electrode when the cell is in water shortage (shelkhin a B, Bushnell C L, pien s s.air-cooled, hydrogen-air fuel cell [ P ]. U.S. patent:5972530,1999.). Adalhart employs hydrophilic silica gel, high surface area alumina or a mixture thereof deposited on the flow field surface of a bipolar plate to make the side surface of the flow field surface of the bipolar plate hydrophilic and store water (Adlhart. Fuel cell system utilization exchange membranes and bipolar plates [ P ]. U.S. patent:4175165,1979.). Koncar et al improved the flow field material based on this study by mixing hydrophilic inorganic oxide particles with graphite powder and resin and press molding to achieve hydrophilicity on the flow channel side of the bipolar plate (Koncar G J, Marianowshi L G.Proton exchange membrane fuel cell separator plate [ P ]. U.S. patent:5942347,1999.).
The porous carbon material is a network structure material formed by a carbon-based skeleton and a mutually penetrating or closed pore structure as a porous carbon structure. The porous carbon has the advantages of ultra-high specific surface area, developed pore structure, low density, high conductivity, good chemical and thermal stability and the like, and has wide application prospects in the fields of macromolecule adsorption, fuel cells, electrocatalysis, hydrogen storage, double electric layer capacitance and the like. Recent attempts to effectively increase the power density and current density of PEMFCs by karthikeeyan et al by filling porous carbon materials into the ridge locations of bipolar plate flow fields have relied on porous carbon being able to effectively wick excess water that accumulates on the surface of the flow channels (karthikeeyan P, variable R J, Muthukumar m. experimental introduction on not less and zigzag porous injectors on the surface of the rib of the flow channel for performance enhancement in PEMFC [ J ]. International Journal of Hydrogen Energy,2015,40(13): 4641-. However, the method has complicated steps and high requirements on sintering temperature and atmosphere, and is not favorable for large-scale industrial application.
Disclosure of Invention
The invention aims to realize a high-porosity porous carbon filled fuel cell flow field structure and a preparation method thereof.
In order to achieve the purpose, the technical scheme of the invention is as follows:
a fuel cell flow field structure filled with high-porosity porous carbon is characterized in that a flow channel of a bipolar plate of a fuel cell is filled with the high-porosity porous carbon structure; wherein the porosity of the porous carbon is 50% -90%. The porous carbon is filled into the flow channel of the bipolar plate, the adding amount is arbitrary, generally 10-100% of the volume of the flow channel, and the flow channel filled with the porous carbon is usually ground to be flat.
The flow channel of the fuel cell bipolar plate is filled with a porous carbon structure with high porosity, and the porous carbon is used as a hydrophilic layer to replace air so as to enhance the water management capability of the bipolar plate.
The porous carbon is:
1) weighing and uniformly mixing coarse and fine carbon fibers and thermoplastic phenolic resin to serve as a carbon source precursor, wherein the mass ratio of the thermoplastic phenolic resin to the coarse and fine carbon fibers is 1% -5%;
2) adding a mixed solution of water and ethanol into the precursor prepared in the step 1), uniformly mixing the system, and sintering at a constant temperature of 50-200 ℃ to obtain the porous carbon with the porosity of 50-90%.
The coarse carbon fiber and the fine carbon fiber are mixed according to the weight ratio of 1:10-1: 2; wherein the fine carbon fiber is 50-500 mesh carbon fiber powder, and the coarse carbon fiber is 1-10 mm short carbon fiber.
A preparation method of a fuel cell flow field structure filled with high-porosity porous carbon comprises the following steps:
1) weighing and uniformly mixing coarse and fine carbon fibers and thermoplastic phenolic resin to serve as a carbon source precursor, wherein the mass ratio of the thermoplastic phenolic resin to the coarse and fine carbon fibers is 1% -5%;
2) adding a mixed solution of water and ethanol into the precursor prepared in the step 1) to uniformly mix the system;
3) kneading the mixture obtained in the step 2) into mud, filling the mud into a flow channel of a bipolar plate, and sintering at a constant temperature of 50-200 ℃ for 5-30 minutes;
4) and 3) taking out the fired bipolar plate obtained in the step 3), and cooling at room temperature to obtain the high-porosity porous carbon filled fuel cell flow field structure.
The coarse carbon fiber and the fine carbon fiber are mixed according to the weight ratio of 1:10-1: 2; wherein the fine carbon fiber is 50-500 mesh carbon fiber powder, and the coarse carbon fiber is 1-10 mm short carbon fiber.
The flow field material of the bipolar plate adopts graphite, stainless steel or titanium material.
The invention has the following characteristics:
1. the novel fuel cell flow field processing method is characterized in that a porous carbon structure with high porosity is filled in a fuel cell flow channel, and the excellent wettability of the porous carbon is utilized to enhance the water management capability of the fuel cell bipolar plate.
2. Compared with the conventional preparation method of the porous carbon structure, the preparation method of the porous carbon structure provided by the invention is quicker, the conditions are milder, and the selection of experimental conditions is more flexible. The method specifically comprises the following steps: 1) carbon fiber is directly used as a carbon source, phenolic resin is used as a cross-linking agent, and a porous carbon structure with excellent wettability is rapidly prepared under a low-temperature condition; 2) the porosity of the porous carbon is increased by a method of combining ethanol, deionized water and thick and thin carbon fibers.
3. The method has the advantages of simple equipment, common chemical raw materials for synthesizing the materials, low cost, simple and quick preparation process, mild conditions and suitability for large-scale industrial production.
Drawings
Fig. 1 is a microstructure diagram of porous carbon provided in an embodiment of the present invention.
Fig. 2 is a microstructure diagram of porous carbon provided in an embodiment of the present invention.
Fig. 3 is a schematic diagram of a porous carbon filled fuel cell flow field provided by an embodiment of the present invention.
Detailed Description
According to the invention, the porous carbon is filled in the flow channel of the fuel cell bipolar plate to enhance the water management capability of the fuel cell bipolar plate, and the porous carbon structure with good wettability, high strength and high porosity can be prepared at low temperature and in short time in the gelation stage of the phenolic resin in the preparation of the porous carbon.
The porous carbon structure with good wettability, high strength and high porosity is prepared by utilizing the gelation stage of the phenolic resin, and the porous carbon is filled in the flow channel of the bipolar plate of the fuel cell so as to enhance the water management capability of the bipolar plate. Compared with the conventional preparation method of the porous carbon structure, the method provided by the invention is quicker, milder in conditions and more flexible in selection of experimental conditions. The method specifically comprises the following steps: 1) carbon fiber is directly used as a carbon source, phenolic resin is used as a cross-linking agent, and a porous carbon structure with excellent wettability is rapidly prepared under a low-temperature condition; 2) the porosity of the porous carbon is increased by a method of combining ethanol, deionized water and thick and thin carbon fibers. The method has the advantages of simple equipment, common chemical raw materials for synthesizing the materials, low cost, simple and quick preparation process, mild conditions and suitability for large-scale industrial production.
The following detailed description of embodiments of the invention refers to the accompanying drawings. It should be understood that the detailed description and specific examples, while indicating the present invention, are given by way of illustration and explanation only, not limitation.
The present invention will be described in detail below by way of examples.
In the following examples, the reagents used are as follows: the carbon fiber is purchased from Shanghai Kargi specialization engineering technology, Inc., and the phenolic resin and the ethanol are purchased from national medicine group chemical reagent, Inc.
The porous carbon microtopography was determined by characterization with a scanning electron microscope (SEM, Hitachi-S4800, acceleration voltage typically 10 kV).
Example 1
Weighing 2g of carbon fiber powder with 300 meshes and 0.07g of thermoplastic phenolic resin, uniformly mixing the carbon fiber powder and the thermoplastic phenolic resin by using a mortar, adding 1ml of deionized water and 1ml of ethanol, grinding the mixture into mud by using the mortar, and cutting the mud into pieces with the same size of 0.5cm3The cube is placed in a drying oven at 150 ℃ to be fired for 15 minutes, and then the cube is taken out and placed at room temperature to be cooled, so that porous carbon is obtained for later use, and the porosity of the obtained porous carbon is 54%.
Example 2
Weighing 2g of carbon fiber powder with 300 meshes and 0.05g of thermoplastic phenolic resin, uniformly mixing the carbon fiber powder and the thermoplastic phenolic resin by using a mortar, adding 1ml of deionized water and 1ml of ethanol, grinding the mixture into mud by using the mortar, and cutting the mud into pieces with the same size of 0.5cm3The cube is placed in a drying oven at 150 ℃ to be fired for 15 minutes, and then the cube is taken out and placed at room temperature to be cooled, so that the porous carbon is obtained for later use; the resulting porous carbon porosity was 56% with increasing phenolic resin content.
Example 3
Weighing 2g of carbon fiber powder with 300 meshes and 0.03g of thermoplastic phenolic resin, uniformly mixing the carbon fiber powder and the thermoplastic phenolic resin by using a mortar, adding 1ml of deionized water and 1ml of ethanol, grinding the mixture into mud by using the mortar, and cutting the mud into pieces with the same size of 0.5cm3The cube is then placed in an oven at 150 ℃ to be fired for 15 minutes, and then taken out and placed at room temperature to be cooled, so that the porous carbon (see figure 1) is obtained for later use; it can be seen from fig. 1 that the porous carbon pore channel obtained is clearly visible, with a porosity of 60%.
Example 4
Weighing 2g of carbon fiber powder with 300 meshes, 0.05g of thermoplastic phenolic resin and 0.4g of carbon fiber with 3mm, uniformly mixing by using a mortar, adding 1ml of deionized water and 1ml of ethanol, grinding into mud by using the mortar, and cutting into pieces of 0.5cm3The cube is then fired in an oven at 150 ℃ for 15 minutes, and then taken out and cooled at room temperature to obtain the porous carbon (see fig. 2) for later use.
It can be seen from fig. 2 that the porous carbon obtained exhibited a pore structure of larger pore size, with a porosity of 68%.
Example 5
Weighing 2g of carbon fiber powder with 300 meshes, 0.05g of thermoplastic phenolic resin and 0.6g of carbon fiber with 3mm, uniformly mixing by using a mortar, adding 1ml of deionized water and 1ml of ethanol, and then usingGrinding into paste with mortar, and cutting into 0.5cm3The cube is placed in a drying oven at 150 ℃ to be fired for 15 minutes, and then the cube is taken out and placed at room temperature to be cooled, so that the porous carbon is obtained for later use; the porosity of the obtained porous carbon is improved to 74%.
Example 6
Weighing 2g of carbon fiber powder with 300 meshes, 0.05g of thermoplastic phenolic resin and 0.8g of carbon fiber with 3mm, uniformly mixing by using a mortar, adding 1ml of deionized water and 1ml of ethanol, grinding into mud by using the mortar, and cutting into pieces of 0.5cm3The cube is placed in a drying oven at 150 ℃ to be fired for 15 minutes, and then the cube is taken out and placed at room temperature to be cooled, so that the porous carbon is obtained for later use; the porosity of the obtained porous carbon is further improved to 80%.
The porosity of the porous carbon obtained above was tested by the suction infiltration method:
the porosity of a porous material is the fraction of pores in the total volume of the material. This parameter is usually denoted by Φ:
wherein VpIs the effective pore volume, V0Is the total volume.
Suction and infiltration method: the porous materials are easy to absorb water due to the loose porous structure on the surface.
In such a case, if a piece of porous carbon is submerged in water under vacuum, after a sufficient period of time, the pore space will be completely filled with water, and the mass of the saturated water sample is:
m＝m0+ρwVpformula (2)
Wherein m is0Is the dry mass of the sample, pwIs the density of the water, thus yielding the effective pore volume:
then, there are:
from the above described method, the porosity statistics of Table 1 for examples 1-6 were obtained.
TABLE 1
The number of statistics for each example was 5 or more.
As shown in table 1, the porosity of the porous carbon gradually increases with the decrease of the content of the phenolic resin, and the addition of the coarse carbon fibers significantly increases the porosity of the porous carbon; but the content of the phenolic resin cannot be too low, otherwise, the strength of the porous carbon structure is not enough, and the porous carbon structure is easy to collapse; too high a level can result in plugging of the channels and reduced porosity. Too high a content of coarse carbon fibers may also cause instability of the porous carbon structure.
Example 7
Weighing 2g of carbon fiber, 0.05g of thermoplastic phenolic resin and 0.8g of 3mm carbon fiber, uniformly mixing the carbon fiber, the thermoplastic phenolic resin and the 3mm carbon fiber by using a mortar, adding 1ml of deionized water and 1ml of ethanol, grinding the mixture into a mud shape by using the mortar, uniformly coating the mud shape in a flow channel of a titanium bipolar plate flow field, then placing the mud shape in a 150 ℃ oven for firing for 15 minutes, taking out the baked mud shape, and placing the baked mud shape in a room temperature for cooling to obtain a flow field structure of the porous.
Example 8
Weighing 10g of carbon fiber, 0.25g of thermoplastic phenolic resin and 4g of 3mm carbon fiber, uniformly mixing the carbon fiber, the thermoplastic phenolic resin and the carbon fiber with a mortar, adding 5ml of deionized water and 5ml of ethanol, grinding the mixture into a mud shape by the mortar, uniformly coating the mud shape in a flow channel of a titanium bipolar plate flow field, then placing the mud shape in a 150 ℃ oven for firing for 15 minutes, taking out the mud shape, and placing the baked mud shape in a room temperature for cooling to obtain a porous carbon filled fuel cell flow field structure (see figure 3) for later.
The optical diagram of fig. 3 shows that the porous carbon structure is uniformly filled in the flow field flow channel, and has strong strength and stable structure.
The fuel cell flow field structure filled with the porous carbon has excellent hydrophilic characteristic, can effectively absorb redundant water accumulated on the surface of a flow channel through capillary action, discharges redundant water in the cell, and avoids the phenomenon of cathode flooding. In addition, the high conductivity of the porous carbon does not cause the increase of the internal resistance of the battery. Meanwhile, the invention is suitable for all flow field structures.
The preferred embodiments of the present invention have been described in detail, however, the present invention is not limited to the specific details of the above embodiments, and various simple modifications may be made to the technical solution of the present invention within the technical idea of the present invention, and these simple modifications are within the protective scope of the present invention.
It should be noted that the various technical features described in the above embodiments can be combined in any suitable manner without contradiction, and the invention is not described in any way for the possible combinations in order to avoid unnecessary repetition.
In addition, any combination of the various embodiments of the present invention is also possible, and the same should be considered as the disclosure of the present invention as long as it does not depart from the spirit of the present invention.
Claims (1)
1. A preparation method of a high-porosity porous carbon filled proton exchange membrane fuel cell flow field structure is characterized by comprising the following steps:
1) weighing and uniformly mixing coarse and fine carbon fibers and thermoplastic phenolic resin to serve as a carbon source precursor, wherein the mass ratio of the thermoplastic phenolic resin to the coarse and fine carbon fibers is 1% -5%;
2) adding a mixed solution of water and ethanol into the precursor prepared in the step 1) to uniformly mix the system;
3) kneading the mixture obtained in the step 2) into mud, filling the mud into a flow channel of a bipolar plate, and sintering at the constant temperature of 50-200 ℃ for 5-30 minutes;
4) taking out the fired bipolar plate obtained in the step 3), placing the bipolar plate at room temperature, and cooling to obtain a high-porosity porous carbon filled proton exchange membrane fuel cell flow field structure;
the coarse carbon fiber and the fine carbon fiber are mixed according to the weight ratio of 1:10-1: 2; wherein the fine carbon fiber is 50-500 mesh carbon fiber powder, and the coarse carbon fiber is 1-10 mm short carbon fiber;
the flow field material of the bipolar plate adopts graphite, stainless steel or titanium material;
the flow field structure of the proton exchange membrane fuel cell is that a porous carbon structure with high porosity is filled in a flow channel of a bipolar plate of the proton exchange membrane fuel cell, and excess water accumulated on the surface of the flow channel is absorbed through capillary action to be discharged; wherein the porosity of the porous carbon is 50% -90%.
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| CN1201554A (en) * | 1995-10-06 | 1998-12-09 | 陶氏化学公司 | Flow field structures for membrane electrode assemblies of fuel cells |
| CN101258631A (en) * | 2005-09-07 | 2008-09-03 | 丰田自动车株式会社 | Tubular solid polymer fuel cell comprising a rod-shaped current collector with peripheral glas flow channels and production method thereof |
| CN103985886A (en) * | 2013-02-07 | 2014-08-13 | 上海恒劲动力科技有限公司 | Fuel cell netted support bipolar plate and electric pile comprising fuel cell netted support bipolar plate |
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| US6838202B2 (en) * | 2002-08-19 | 2005-01-04 | General Motors Corporation | Fuel cell bipolar plate having a conductive foam as a coolant layer |
| CN1236513C (en) * | 2003-05-22 | 2006-01-11 | 上海交通大学 | High-per formance carbon material preparing method by water-base curtain coating technology |
| CN105742667B (en) * | 2016-04-19 | 2018-06-08 | 武汉理工大学 | A kind of cathode flow field plate biomimetic features for improving fuel cell drainage performance |
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Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1201554A (en) * | 1995-10-06 | 1998-12-09 | 陶氏化学公司 | Flow field structures for membrane electrode assemblies of fuel cells |
| CN101258631A (en) * | 2005-09-07 | 2008-09-03 | 丰田自动车株式会社 | Tubular solid polymer fuel cell comprising a rod-shaped current collector with peripheral glas flow channels and production method thereof |
| CN103985886A (en) * | 2013-02-07 | 2014-08-13 | 上海恒劲动力科技有限公司 | Fuel cell netted support bipolar plate and electric pile comprising fuel cell netted support bipolar plate |
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| Experimental investigation on uniform and zigzag positioned porous inserts on the rib surface of cathode flow channel for performance enhancement in PEMFC;P. Karthikeyan等;《International Journal of Hydrogen Energy》;20150226;第40卷;第4641-4648页 * |
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