CN112952166B - Membrane electrode and battery with wetting function and high mass transfer - Google Patents
Membrane electrode and battery with wetting function and high mass transfer Download PDFInfo
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- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
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Abstract
The invention provides a membrane electrode and a battery with a wetting function and high mass transfer, wherein the membrane electrode comprises proton exchange membranes which are arranged in sequence; a cathode wetting layer; a cathode catalyst layer; the cathode wetting layer comprises resin and a porous carrier in a mass ratio of 0.7-1.3: 1; the cathode wetting layer is a hydrophilic porous medium for transferring protons; the cathode wetting layer is more hydrophilic than the cathode catalytic layer. The membrane electrode is provided with a cathode wetting layer, the hydrophilicity of the cathode wetting layer is greater than that of the cathode catalyst layer, partial liquid water generated by the cathode catalyst layer can be dragged to form a water-retaining area, the water-retaining area provides better wetting for the membrane and electrolyte, and meanwhile, the established hydraulic gradient can promote the back diffusion of water from the cathode to the anode and slow down the water-deficient state of the anode; compared with the traditional membrane electrode structure, the liquid water reserved in the rest areas of the cathode electrode is reduced to a certain extent, and can provide smaller resistance for oxygen transmission, so that the membrane electrode has a more efficient gas mass transfer function.
Description
Technical Field
The invention belongs to the technical field of membrane electrodes, and particularly relates to a membrane electrode and a battery with a wetting function and high mass transfer.
Background
In recent years, proton exchange membrane fuel cells are widely concerned with the characteristics of high power density, quick start, low emission and the like, and are expected to be used as vehicle power sources to achieve the aims of zero exhaust emission and energy independence expected by the automobile industry. As the technology of proton exchange membrane fuel cells is moved into the application stage, the research direction gradually changes from the initial material development to the aspects of system and structural design (including the structural design of electrodes and cells).
The transmission process inside the proton exchange membrane fuel cell mainly comprises mass transfer phenomena such as transmission of reaction gas and water in a flow channel and a porous electrode, phase change of water, absorption and release of water by a membrane, conduction of protons and electrons and the like, and heat transfer phenomena caused by heat generation and heat absorption such as substance entropy change, electrochemical reaction, ohmic resistance, phase change and the like, and the heat transfer and mass transfer processes under the multi-scale structures are mutually coupled, so that the research on the problem is very complex. Since the last 90 s of the century, researchers have pointed out the importance of hydrothermal transport optimization to improve battery power density and durability and reduce cost, with the central idea being: based on a basic heat and mass transfer mechanism, the multi-component multi-phase transmission process in the fuel cell is optimized, and on the premise of ensuring membrane humidification (reducing resistance), reaction gas transmission and liquid water discharge are accelerated (the electrochemical reaction rate is improved), so that the performance is improved.
With the development of a new generation of high power density galvanic pile, industrialization and basic theory research both put new requirements on water thermal management of fuel cells. On one hand, the work of no external humidification technology development, cold start strategy optimization, dynamic working condition influence research and the like needs to be further developed to meet the increasing development demand; on the other hand, the continuous improvement of the current density greatly increases the nonuniformity of the reactant gas, the temperature and the liquid water distribution, particularly along the direction of the flow channel, so that the electrolyte in the area of the cathode inlet is possibly insufficiently wetted, and the electrode or flow channel is flooded in the area of the outlet, so that the local gas supply is insufficient, and the performance and the service life of the battery are influenced. The structural design of the membrane electrode has the following contradictions: the membrane needs the electrodes to retain enough water for wetting so as to improve proton conductivity, while the reaction gas transmission needs smooth pore channels so as to support electrode reaction under high current density, and the conflict of the two requirements on water is the difficulty of designing and optimizing the membrane electrode in the aspect of hydrothermal management.
Disclosure of Invention
In view of the above, the present invention aims to provide a membrane electrode and a cell having a wetting function and high mass transfer, wherein the membrane electrode has a relatively high efficiency gas mass transfer function.
The invention provides a membrane electrode with a wetting function and high mass transfer, which comprises proton exchange membranes arranged in sequence;
a cathode wetting layer;
a cathode catalyst layer;
the cathode wetting layer comprises resin and a porous carrier in a mass ratio of 0.7-1.3: 1; the cathode wetting layer is a hydrophilic porous medium for transferring protons;
the cathode wetting layer is more hydrophilic than the cathode catalytic layer.
Preferably, the cathode wetting layer has a thickness of 1 to 10 μm.
Preferably, the resin is a perfluorosulfonic acid resin.
Preferably, the EW value of the resin is 600-1200 g/mol.
Preferably, the support is a carbon support.
Preferably, the thickness of the cathode catalyst layer is 9-11 μm.
The membrane electrode also comprises a microporous layer and a gas diffusion layer which are arranged on the other side of the cathode catalyst layer, and an anode catalyst layer, an anode microporous layer and an anode gas diffusion layer which are arranged on the other side of the proton exchange membrane;
preferably, the thickness of the anode catalyst layer is 2-3 μm; the thickness of the anode microporous layer and the thickness of the cathode microporous layer are respectively 25-32 mu m; the thickness of the anode gas diffusion layer and the thickness of the cathode gas diffusion layer are 120-160 mu m respectively.
Preferably, the cathode wetting layer is free of catalyst.
The invention provides a battery, which comprises the membrane electrode in the technical scheme.
The invention provides a membrane electrode with a wetting function and high mass transfer, which comprises proton exchange membranes arranged in sequence; a cathode wetting layer; a cathode catalyst layer; the cathode wetting layer comprises resin and a porous carrier in a mass ratio of 0.7-1.3: 1; the cathode wetting layer is a hydrophilic porous medium for transferring protons; the cathode wetting layer is more hydrophilic than the cathode catalytic layer. The membrane electrode provided by the invention is provided with the cathode wetting layer, the hydrophilicity of the cathode wetting layer is greater than that of the cathode catalyst layer, partial liquid water generated by the cathode catalyst layer can be dragged to form a water-retaining area, the existence of the water-retaining area provides better wetting for the membrane and electrolyte, and meanwhile, the established hydraulic gradient can promote the back diffusion of water from the cathode to the anode and slow down the water-deficient state of the anode; compared with the traditional membrane electrode structure, the liquid water reserved in the rest areas of the cathode electrode is reduced to a certain extent, and can provide smaller resistance for oxygen transmission, so that the membrane electrode has a more efficient gas mass transfer function.
Drawings
FIG. 1 is a schematic diagram of a cathode structure of a membrane electrode provided by the present invention;
FIG. 2 is a graph comparing cell performance and impedance obtained in example 1 of the present invention, with WL representing the cathode wetting layer;
FIG. 3 is a comparison graph of the hydrophilic-hydrophobic properties of each layer in the membrane electrode prepared in example 1 of the present invention;
FIG. 4 is a graph comparing voltage losses for cells prepared in example 1 of the present invention, WL representing the cathode wetting layer;
FIG. 5 is a graph showing a comparison of liquid water saturation for each layer of the membrane electrode prepared in example 1 of the present invention, and a current density of 2000mA/cm2And WL denotes a cathode wetting layer.
Detailed Description
The invention provides a membrane electrode with a wetting function and high mass transfer, which comprises proton exchange membranes arranged in sequence;
a cathode wetting layer;
a cathode catalyst layer;
the cathode wetting layer comprises resin and a porous carrier in a mass ratio of 0.7-1.3: 1; the cathode wetting layer is a hydrophilic porous medium for transferring protons;
the cathode wetting layer is more hydrophilic than the cathode catalytic layer.
The invention arranges a cathode wetting layer which is a hydrophilic porous medium for transferring protons; it has the functions of moistening electrolyte and proton exchange membrane, and is favorable to draining water and has high efficiency gaseous mass transfer function. The membrane electrode can relieve the conflict of membrane wetting and reaction gas transmission on water requirement to a certain extent, and realizes the functional zoning of the membrane and the reaction gas.
Referring to fig. 1, fig. 1 is a schematic structural diagram of a cathode of a membrane electrode with a wetting function and high mass transfer provided by the present invention.
The membrane electrode provided by the invention comprises a proton exchange membrane; in one embodiment, the thickness of the membrane is 10 μm, and the EW of the membrane is 1000 g/mol.
In the present invention, the thickness of the cathode wetting layer is 1 to 10 μm, preferably 1 to 7 μm, and more preferably 1 to 4 μm. The cathode wetting layer is free of catalyst and does not take charge of electrochemical reaction.
In the present invention, the resin in the cathode wetting layer is preferably a perfluorosulfonic acid resin; the EW value of the resin is preferably 600 to 1200g/mol, more preferably 600 to 1000g/mol, and most preferably 600 to 900 g/mol.
In a specific embodiment, the resin used in the cathode wetting layer has an EW value of 900 g/mol;
in the present invention, the porous support in the cathode wetting layer is preferably a carbon support, and may be a gel support. In a specific embodiment, the support is a carbon support.
The mass ratio of the resin to the porous carrier is 0.7-1.3: 1, preferably 0.9-1.3: 1, and more preferably 1.1-1.3: 1. In a specific embodiment, the carbon content in the cathode wetting layer is 0.025mg/cm2(ii) a The mass ratio of the resin to the porous carrier was 1: 1.
The membrane electrode provided by the invention comprises a cathode catalyst layer; the thickness of the cathode catalyst layer is 5 to 15 μm, preferably 9 to 11 μm. The cathode catalyst layer comprises a carbon carrier, platinum particles and resin; the platinum loading in the cathode catalyst layer is 0.25mg/cm2(ii) a The platinum mass fraction of the catalyst in the cathode catalyst layer is 50%; the electrochemical active area of the cathode catalyst layer is 50m2(ii)/g; the EW value of the resin in the cathode catalyst layer is 900 g/mol; the mass ratio of the resin to the carbon support was 1: 1.
The membrane electrode provided by the invention also comprises a cathode microporous layer and a cathode gas diffusion layer which are arranged on the other side of the cathode catalyst layer, and an anode catalyst layer, an anode microporous layer and an anode gas diffusion layer which are arranged on the other side of the proton exchange membrane; the thickness of the cathode microporous layer and the thickness of the anode microporous layer are respectively 20-60 micrometers, and preferably 25-32 micrometers; the thicknesses of the cathode gas diffusion layer and the anode gas diffusion layer are 100-200 mu m, preferably 120-160 mu m.
In specific implementation, the thickness of the anode catalyst layer is preferably 2-3 μm. The anode catalyst layer comprises a carbon carrier, platinum particles and resin; the platinum loading in the anode catalyst layer is 0.05mg/cm2(ii) a The mass fraction of platinum in the anode catalyst layer is 50%; the electrochemical active area of the anode catalyst layer is 50m2(ii)/g; the EW value of the resin in the anode catalyst layer is 900 g/mol; the mass ratio of the resin to the carbon support was 1: 1.
The cathode microporous layer and the anode microporous layer had a thickness of 25 μm, a porosity of 0.3, and an average diameter of pores of 60 nm.
The cathode and anode gas diffusion layers had a thickness of 140 μm, a porosity of 0.75 and a dry diffusion factor of 3.5.
In addition, due to the existence of the water retention area, the cathode catalyst layer, the microporous layer and the gas diffusion layer can be further designed into a more hydrophobic high mass transfer structure by adjusting the porosity, the pore diameter, adding a hydrophobic agent and the like without worrying about the wetting of the proton exchange membrane. In addition, the addition of the cathode wetting layer prolongs the proton conduction path, resulting in additional proton conduction losses, which can be reduced by optimizing the cathode wetting layer thickness, resin content, and the choice of high proton conductivity resin.
The invention provides a battery, which comprises the membrane electrode in the technical scheme.
For further illustration of the present invention, a membrane electrode and a cell having a wetting function and a high mass transfer according to the present invention will be described in detail with reference to examples, which should not be construed as limiting the scope of the present invention.
Comparative example
Conventional membrane electrode structures typically include a proton exchange membrane, a cathode and anode catalyst layer, a cathode and anode microporous layer, and an anode and cathode gas diffusion layer, wherein the microporous layer is typically attached to one side of the gas diffusion layer. Membrane electrodes are classified into ccm (purified membrane) type and gde (gas diffusion electrode) type membrane electrodes according to the position of the cathode and anode catalyst layers. The comparative example prepared a CCM type membrane electrode, the main steps were as follows:
1. preparing catalyst slurry: mixing a catalyst, a resin solution, alcohol and water according to a certain proportion, and uniformly dispersing by ultrasonic oscillation;
CCM preparation: spraying the catalyst slurry on a proton exchange membrane under an ultrasonic condition, and drying and forming;
3. frame pressfitting: pressing the CCM and the membrane electrode frame;
4. carbon paper lamination: and (3) attaching the carbon paper to the two sides of the CCM by hot pressing or other methods.
Example 1
On the basis of a comparative example, the following two procedures are firstly carried out:
1. preparing a wetting layer slurry: mixing a carbon carrier, a resin solution, alcohol and water according to a certain proportion, and uniformly dispersing by ultrasonic oscillation;
2. coating of a wetting layer: spraying the slurry of the wetting layer on the proton exchange membrane under the ultrasonic condition, and drying and forming;
after the preparation of the membrane electrodes of the comparative example and the example 1 is finished, matching proper bipolar plates and clamps, and respectively preparing single cells with certain assembly force;
the cell prepared in example 1 includes a cathode gas diffusion layer, a cathode microporous layer, a cathode catalytic layer, a cathode wetting layer, a proton exchange membrane, an anode catalytic layer, an anode microporous layer, and an anode gas diffusion layer, which are sequentially disposed;
the cell prepared in the comparative example included a cathode gas diffusion layer, a cathode microporous layer, a cathode catalytic layer, a proton exchange membrane, an anode catalytic layer, an anode microporous layer, and an anode gas diffusion layer, which were sequentially disposed.
FIG. 2 is a graph comparing cell performance and impedance obtained in example 1 of the present invention, with WL representing the cathode wetting layer; as can be seen from fig. 2, under the relatively humid operating conditions in table 1, the output voltage of the conventional membrane electrode structure (without the wetting layer) is sharply reduced under the high current density condition, while the output voltage of the membrane electrode structure with the cathode wetting layer is significantly reduced under the high current density condition.
TABLE 1 operating conditions of the cell
| |
80 | ℃ |
| Anode back pressure | 50 | kPa |
| Cathode back pressure | 50 | kPa |
| Anode gas | Humidified hydrogen gas | / |
| Cathode gas | Humidifying air | / |
| Anode intake metering ratio | 2.0 | / |
| Cathode intake air metering ratio | 2.0 | / |
| Relative humidity of |
100 | ％RH |
| Cathode inlet |
100 | ％RH |
Table 2 shows the parameters of each layer structure in the membrane electrode
Referring to fig. 3, fig. 3 shows the hydrophilicity and hydrophobicity of each layer calculated based on the structural parameters of table 2. Note that the degree of hydrophilicity and hydrophobicity herein is defined by the magnitude of capillary pressure (related to contact angle, permeability, porosity, pore size, liquid water saturation, etc.), and not based on pure contact angle values, the smaller the capillary pressure, the more hydrophilic the layer appears to be. As can be seen from fig. 3, the cathode wetting layer of the present embodiment is designed to be more hydrophilic than the catalytic layer, so as to achieve the purposes of drawing liquid water to form a "water retention zone" and improving oxygen mass transfer of the electrode.
Referring to fig. 4, fig. 4 is a graph showing the voltage loss of each battery obtained in example 1 of the present invention. As can be seen from fig. 4, the sharp decrease of the high electrical performance of the conventional membrane electrode structure cell in fig. 2 is mainly caused by the rapid increase of mass transfer loss, which indicates that the cell has a serious mass transfer problem, while the mass transfer loss of the membrane electrode added to the cathode wetting layer increases at a significantly slower rate.
Referring to FIG. 5, FIG. 5 shows a current density of 2000mA/cm2Next, a comparison graph of the liquid water saturation obtained in example 1 of the present invention is shown. As can be seen from fig. 5, the accumulation of liquid water in the cathode catalyst layer in the conventional membrane electrode structure aggravates the problem of oxygen mass transfer to some extent.
As can be seen from the liquid water saturation distribution diagram in fig. 5, after the cathode wetting layer is added, part of the liquid water generated by the cathode catalytic layer is dragged to the cathode wetting layer under the action of capillary pressure to form a "water retention area", and as the drainage flow rate decreases, the liquid water retained by the cathode catalytic layer, the microporous layer and the gas diffusion layer decreases to a certain extent compared with the original traditional membrane electrode structure. The presence of the "water retention zone" provides better wetting of the membrane and electrolyte, while the established hydraulic gradient can promote back diffusion of water from the cathode to the anode, slowing the water-deficient state of the anode, as can be seen from fig. 2 and 4, the cell impedance with the cathode wetting layer added is lower and the ohmic loss is less under high current density conditions. The reduced amount of liquid water in the cathode catalyst layer, the microporous layer and the gas diffusion layer provides less resistance to oxygen transfer, and as can be seen from fig. 2 and 4, the mass transfer loss under the high current density working condition is reduced by about 50mV after the cathode wetting layer is added.
From the above embodiments, the invention provides a membrane electrode with a wetting function and high mass transfer, which comprises proton exchange membranes arranged in sequence; a cathode wetting layer; a cathode catalyst layer; the cathode wetting layer comprises resin and a porous carrier in a mass ratio of 0.7-1.3: 1; the cathode wetting layer is a hydrophilic porous medium for transferring protons; the cathode wetting layer is more hydrophilic than the cathode catalytic layer. The membrane electrode provided by the invention is provided with the cathode wetting layer, the hydrophilicity of the cathode wetting layer is greater than that of the cathode catalyst layer, partial liquid water generated by the cathode catalyst layer can be dragged to form a water-retaining area, the existence of the water-retaining area provides better wetting for the membrane and electrolyte, and meanwhile, the established hydraulic gradient can promote the back diffusion of water from the cathode to the anode and slow down the water-deficient state of the anode; compared with the traditional membrane electrode structure, the liquid water reserved in the rest areas of the cathode electrode is reduced to a certain extent, and can provide smaller resistance for oxygen transmission, so that the membrane electrode has a more efficient gas mass transfer function.
The foregoing is only a preferred embodiment of the present invention, and it should be noted that, for those skilled in the art, various modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.
Claims (7)
1. A membrane electrode with wetting function and high mass transfer comprises proton exchange membranes arranged in sequence;
a cathode wetting layer; the thickness of the cathode wetting layer is 1-10 mu m;
a cathode catalyst layer; the thickness of the cathode catalyst layer is 5-15 mu m;
the cathode wetting layer is a hydrophilic porous medium for transferring protons, and comprises resin and a porous carrier in a mass ratio of 0.7-1.3: 1; the resin is perfluorosulfonic acid resin, and the EW value of the resin is 600-1200 g/mol; the porous carrier is a carbon carrier or a gel carrier;
the cathode wetting layer is more hydrophilic than the cathode catalytic layer;
the proton exchange membrane further comprises a cathode microporous layer and a cathode gas diffusion layer which are arranged on the other side of the cathode catalytic layer, and an anode catalytic layer, an anode microporous layer and an anode gas diffusion layer which are arranged on the other side of the proton exchange membrane.
2. The membrane electrode according to claim 1, wherein the cathode catalyst layer comprises a carbon support, platinum particles and a resin, wherein the mass ratio of the resin to the carbon support is 1:1, and the platinum loading is 0.25mg/cm2The electrochemical active area of the cathode catalyst layer is 50m2/g。
3. The membrane electrode according to claim 1, wherein the thickness of the anode catalyst layer is 2 to 3 μm, and the thickness of the anode microporous layer and the thickness of the cathode microporous layer are 20 to 60 μm respectively; the thickness of the anode gas diffusion layer and the thickness of the cathode gas diffusion layer are both 100-200 mu m.
4. The membrane electrode assembly according to claim 3, wherein the anode catalytic layer comprises a carbon support, platinum particles, and a resin; the platinum loading capacity in the anode catalyst layer is 0.05mg/cm2(ii) a The electrochemical active area of the anode catalyst layer is 50m2(ii)/g; the mass ratio of the resin to the carbon support is 1: 1.
5. The membrane electrode of claim 3, wherein the cathode microporous layer and the anode microporous layer each have a thickness of 25 μm, a porosity of 0.3, and an average diameter of micropores of 60 nm.
6. The membrane electrode of claim 3, wherein the cathode gas diffusion layer and the anode gas diffusion layer each have a thickness of 140 μm, a porosity of 0.75, and a dry state diffusion factor of 3.5.
7. A battery comprising the membrane electrode of any one of claims 1 to 6.
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