Source: https://patents.google.com/patent/EP1063717A2/en
Timestamp: 2020-07-12 14:19:29+00:00
Document Index: 104410718

Matched Legal Cases: ['art 24', 'art 24', 'art 211', 'art 212', 'art 211', 'art 212', 'art 24', 'art 24', 'art 24', 'art 24', 'art 115', 'art 115', 'art 115', 'art.\n4', 'art.\n5', 'art 115', 'art 115', 'art.\n4']

EP1063717A2 - Stable and high-performance fuel cell - Google Patents
Stable and high-performance fuel cell Download PDF
EP1063717A2
EP1063717A2 EP00113292A EP00113292A EP1063717A2 EP 1063717 A2 EP1063717 A2 EP 1063717A2 EP 00113292 A EP00113292 A EP 00113292A EP 00113292 A EP00113292 A EP 00113292A EP 1063717 A2 EP1063717 A2 EP 1063717A2
EP00113292A
EP1063717B1 (en
EP1063717A3 (en
1999-06-22 Priority to JP17608499 priority
2000-04-21 Priority to JP2000121616 priority
2000-06-21 Application filed by Sanyo Electric Co Ltd filed Critical Sanyo Electric Co Ltd
2000-12-27 Publication of EP1063717A2 publication Critical patent/EP1063717A2/en
2004-03-17 Publication of EP1063717A3 publication Critical patent/EP1063717A3/en
2011-09-28 Publication of EP1063717B1 publication Critical patent/EP1063717B1/en
239000000446 fuel Substances 0.000 title claims abstract description 66
239000007789 gases Substances 0.000 claims abstract description 144
239000007800 oxidant agent Substances 0.000 claims abstract description 92
239000003054 catalyst Substances 0.000 claims abstract description 68
229920005597 polymer membrane Polymers 0.000 claims abstract description 64
230000035699 Permeability Effects 0.000 claims abstract description 59
239000000203 mixtures Substances 0.000 claims description 55
OKTJSMMVPCPJKN-UHFFFAOYSA-N carbon Chemical compound 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230000002940 repellent Effects 0.000 claims description 18
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239000002737 fuel gas Substances 0.000 description 29
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239000004812 Fluorinated ethylene propylene Substances 0.000 description 6
WUOACPNHFRMFPN-UHFFFAOYSA-N Terpineol Chemical compound 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CC1=CCC(C(C)(C)O)CC1 WUOACPNHFRMFPN-UHFFFAOYSA-N 0.000 description 4
The object of the present invention is to provide a fuel cell including a cell that is formed by sandwiching a solid polymer membrane between an anode and a cathode that generates electricity with stability and high performance by evenly moistening the solid polymer membrane. For this purpose, in a gas diffusion layer 24, which is positioned adjacent to a cathode catalyst layer 22, the content of fluororesin in an area on the side of the entrance for the oxidizer is set to be higher than in another area on the side of the exit so that the water repellency in the entrance side area is higher than in the exit side area. As a result, a water permeation suppressing part 24A, where the water permeability is relatively low, is formed in the area on the entrance side, while a water permeable part 24B, where the water permeability is relatively high, is formed in the area on the exit side.
This application is based on application Nos. 11-176084 and 2000-121616 filed in Japan, the contents of which are hereby incorporated by reference.
BACKGROUND OF THE INVENTION. (1)Field of the Invention
The present invention relates to a fuel cell in which a solid polymer membrane is used as the electrolyte film.
(2)Related Art
In the solid polymer electrolyte fuel cell, the solid polymer membrane 201 is sandwiched between the cathode 210 and the anode 220 in the cell, and electricity is generated by flowing the oxidizer gas (the arrow 231) across the cathode 210 and the fuel gas (the arrow 232) across the anode 220 as shown in Fig. 12. The gas diffusivity in the part 211, which is closer to the entrance for the gas, is set to be smaller than that in the part 212, which is closer to the exit for the gas. The gas diffusivity is adjusted by changing the thickness and the ratio of pores of the gas diffusion layer. More specifically, the gas diffusivity is set relatively small by setting the ratio of pores small or the thickness large in the entrance part 211. On the other hand, the gas diffusivity is set relatively large by setting the ratio of pores large or the thickness small in the exit part 212.
The layer adjusting the water permeability may have the function of a gas diffusion layer by being formed of a conductive, porous material that includes a water repellent. In this case the content of the water repellent in the area closer to the entrance for the oxidizer may be set to be higher than the Content of the water repellent in the area closer to the exit for the oxidizer.
In this case, the water permeability may be adjusted by setting the specific surface area of a first carbon material in the area closer to the entrance for the oxidizer smaller than the specific surface area of a second carbon material in the area closer to the exit for the oxidizer, and by adding the water-repellent material to the carbon material so that water repellency of the mixture layer is higher in the area closer to the entrance for the oxidizer than in the area closer to the exit for the oxidizer.
Fig. 12 shows a conventional fuel cell.
DESCRIPTION OF THE PREFERRED EMBODIMENT (The First Embodiment)
(Structure and Operation of Fuel Cell System)
(Detailed Explanation of Cell Structure)
The fuel gas that is to be supplied to the fuel cell is supplied to the anode catalyst layer 23 via the gas diffusion layer 25. In the anode catalyst layer 23, hydrogen in the fuel gas ionizes and emits electrons (H2 → 2H+ + 2e-). The proton generated here moves towards the cathode catalyst layer 22 in the solid polymer membrane 21. With the move of the proton, the water in the anode catalyst layer 23 also moves towards the cathode catalyst layer 22.
On the other hand, the air is supplied to the cathode catalyst layer 22 via the gas diffusion layer 24. In the catalyst layer 22, oxygen in the air is united with the proton that has moved in the solid polymer membrane 21 to form water (O2 + 2e- + 2H+ → H2O).
(Cell Performance Comparative Experiment)
Solid polymer membrane: perfluorocarbon sulfonic acid Membrane (Nafion 112 film, 12cm x 12cm, 50 µm thick)
Cathode catalyst layer and anode catalyst layer: 10cm x 10cm, 20 µm thick
Gas diffusion layer: 10cm x 10cm, 200 µm thick
For the practical examples 1 to 4, the ratio between the area of the water permeation suppressing part 24A and the area of the water permeable part 24B is 1:1 (50cm2 both).
The amount of fluororesin in the gas diffusion layer 24 at the water permeation suppressing part 24A is set to be 26, 30, 50, and 60w%. At the water permeable part 24B, 25w% in common.
For the practical and comparative examples, the ratio of the amount of fluororesin in the water permeation suppressing part to the amount of fluororesin in the water permeable part in the gas diffusion layer is indicated by A/B in Fig. 1.
Gas diffusion layer on the cathode: for the practical examples 1 to 4, carbon paper (200 µm thick) is moistened in PTFE-dispersed solution. After spraying of the PTFE-dispersed solution on the area corresponding to the water permeation supressing part (5cm x 10cm), the gas diffusion layer is calcinated at 380°C for one hour. Other manufacturing conditions are the same as the practical examples 1 to 4.
As a result, gas diffusion layers are manufactured for the practical examples 1 to 4. The amount of fluororesin is 26, 30, 50, and 60wt% at the water permeation suppressing part and 25wt% at the water permeable part.
The gas diffusion layers on the cathode for the comparative examples 1 and 2 are manufactured by moistening the carbon paper in the PTFE-dispersed solution, in which the PTFE density has been adjusted, and calcinating the carbon paper at 380°C for one hour. Other manufacturing conditions are the same as the practical examples 1 to 4.
Gas diffusion layer on the anode: Carbon paper (200 µm thick) is calcinated at 380°C for one hour after moistened in the PTFE-dispersed solution. As a result, gas diffusion layers on the anode are manufactured with 25wt% fluororesin amount.
The solid polymer membrane is sandwiched between the gas diffusion layers (on the anode and cathode), on which the cathode and anode catalyst layers have been formed, and then hot press is performed on the solid polymer membrane and the cathode and anode catalyst layers on the condition of 150°C-60sec. In this way, a cell is manufactured.
(Cell Voltage Measurement)
Operating temperature in cell: 80°C
Another experiment shows that sufficient water repellency cannot be obtained when the amount of fluororesin in the gas diffusion layer on the cathode at the entrance for air is less than 15wt% and that the gas permeability is extremely degraded when the amount of fluororesin is greater than 90wt%.
As a result, it is preferable to set the amount of fluororesin in the gas diffusion layer on the cathode at the entrance for air within 15 to 90wt%.
The following is an explanation of how the oxidizer gas (air), the fuel gas, and the coolant flow in the cell, unit 100.
(Adjustment of Water Permeability of Mixture Layer 113 And Gas Diffusion Layer 112)
As in the case of the first embodiment, the layer 115 (the gas diffusion layer 112 + the mixture layer 113), which is sandwiched between the cathode catalyst layer 111 and the oxidizer gas channels 131, in the cell unit 100 is composed of a water permeation suppressing part 115A, where water permeability is relatively low, in an fixed area extending from the end on the side of the entrance for oxidizer gas (air), i.e., on the side of the hole 64, and a water permeable part 115B, where the water permeability is relatively high, in the remaining area. In the present embodiment, the water permeability of the layer 115 is adjusted by adjusting the water repellency of the mixture layer 113 adjacent to the cathode catalyst layer 111.
More specifically, the tendency that the amount of water evaporating from the solid polymer membrane 101 is larger at the entrance for air clue to the water concentration gradient in the air passing through the oxidizer gas channels 131 can be repressed. As a result, the solid polymer membrane 101 can be evenly moistened at the entrance and the exit for air.
As in the case of the first embodiment, it is preferable to set the ratio of the area of the water permeation suppressing part 115A to the entire area of the layer 115 within 10 to 90%.
More specifically, the water permeability of the mixture layer 113 at the entrance and exit for air is adjusted by adjusting the specific surface area of the carbon material used at the entrance and exit in the second embodiment. On the other hand, the water permeability is adjusted by changing the ratio of the amount of water-repellent material to the amount of the carbon material in the present embodiment. At the entrance for air, the ratio of the amount of the water-repellent material to the amount of the carbon material is larger than at the exit.
1 ○ A piece of carbon paper (TGP-HO60, Toray industries, Inc.) is cut to a predetermined size.
2 ○ The carbon paper is moistened by FEP (fluorinated ethylene propylene resin) dispersion, mixture of FEP and water, in which the specific gravity has been adjusted. After drying the carbon paper, one-hour heat treatment at 380°C is given to form the gas diffusion layer 112.
3 ○ 10g of carbon black powder having the specific surface area of 700 to 800m2/g and 16.7g of PTFE-dispersed solution having the weight percentage of 60wt% are mixed and dispersed using terpineol to which several cc of surface active agent has been added as the dispersant to generate the mixed paste for the water permeable part.
4 ○ 10g of carbon black powder having the specific surface area of 100 to 150m2/g and 16.7g of PTFE-dispersed solution having the weight percentage of 60wt% are mixed and dispersed using terpineol to which several cc of surface active agent has been added as the dispersant to generate the mixed paste for the water permeation suppressing part.
5 ○ The mixed paste that has been generated in 4 ○ is applied onto the gas diffusion layer 112 in the area corresponding to the water permeation suppressing part 115A. On the other hand, the mixed paste that has been generated in the process 3 ○ is applied onto the gas diffusion layer 112 in the area corresponding to the water permeable part 115B.
6 ○ After drying of the mixed pastes that have been applied onto the gas diffusion layer 112, one-hour heat treatment at 360°C is given to form the mixture layer 113 on the gas diffusion layer 112.
7 ○ The mixed paste of platinum-supporting carbon (the specific surface area of the catalyst support carbon is 200 to 300m2/g) and polymer electrolyte (ion exchange resin) is applied onto the mixture layer 113 to form the cathode catalyst layer 111. As a result, the cathode 110 is formed.
8 ○ The anode 120 is formed in the same manner as the precesses 1 ○ to 7 ○ . Note that one kind of carbon black powder is used for the entire area of the mixture layer 123 in the process for forming the mixture layer 123 for the anode 120.
The cell, unit 100 is manufactured in the same way as the practical example 5. The amount of the PTFE-dispersed solution having the weight percentage of 60wt% that is mixed with 10g of carbon black powder having the specific surface area of 700 to 800m2/g is set as 7.0g when generating the mixed paste for the water permeable part in the process 3 ○ .
The cell unit 100 is manufactured in the same way as the practical example 5. In this case, instead of the carbon black powder having the specific surface area of 700 to 800m2/g, carbon black powder having the specific surface area of 200 to 300m2/g is used when generating the mixed paste for the water permeable part in the process 3 ○ .
The cell unit 100 is manufactured in the same way as the practical example 5. In this case, instead of the carbon black powder having the specific surface area of 100 to 150m2/g, carbon black powder having the specific surface area of 200 to 300m2/g is used when generating the mixed paste for the water permeation suppressing part in the process 4 ○ .
The cell unit is manufactured in the same way as the practical example 5. In this case, carbon black powder having the specific surface area of 200 to 300m2/g is used in the processes 3 ○ and 4 ○ .
The specific surface areas of the carbon black powders used for the practical examples 5 to 8 and the comparative example 3 and the ratios of the carbon black powders to the PTFE are shown in Table 2.
(Table 2) (Practical Example 9)
The cell unit 100 is manufactured in the same way as the practical example 5. In this case, the mixed pastes for the water permeation suppressing part and the water permeable part are generated in the processes 3 ○ and 4 ○ as follows.
3 ○ 10g of carbon black powder having the specific surface area of 200 to 300m2/g and 7g of PTFE-dispersed solution having, the weight percentage of 60wt% are mixed and dispersed using terpineol as the dispersant. Then, several cc of surface active agent is added to and mixed with the mixture to generate the mixed paste for the water permeable part.
4 ○ 10g of carbon black powder having the specific surface area of 200 to 300m2/g and 16.7g of PTFE-dispersed solution having the weight percentage of 60wt% are mixed and dispersed using terpineol as the dispersant. Then, several cc of surface active agent is added to and mixed with the mixture to generate the mixed paste for the water permeation suppressing part.
As in the case of the process 1 ○ , a piece of carbon paper is cut to a predetermined size. Then, the carbon paper is moistened by the FEP dispersion, mixture of FEP and water, in which the specific gravity has been adjusted. After drying the carbon paper, only the water permeable part is moistened by the FEP dispersion. After drying the carbon paper again, one-hour heat treatment at 380°C is given to form the gas diffusion layer 112.
The content of the FEP in the gas diffusion layer 112 that has been formed in this way is 20wt% at the entrance for air. At the exit, the amount is tremendously large, i.e., 50wt%.
(Table 3) (Cell Performance Comparative Experiment 1)
Fig. 9 is a plot showing the result of the experiment. In Fig. 9, the vertical axis indicates the average cell voltage (mV) and the horizontal axis indicates the humidifying temperature of air (°C).
Among the practical examples 5 to 8, the practical example 6 shows the most favorable cell, voltage.
(Cell Performance Comparative Experiment 2)
Figs. 10 and 11 are plots showing the experiment results. In Fig. 10, the vertical axis indicates the average cell voltage (mV) and the horizontal axis indicates the current density (Amp/cm2). In Fig. 21, the vertical axis indicates the average cell voltage (mV) and the horizontal axis indicates the humidifying temperature of air (°C).
In the embodiments, the layer to adjust the water permeability (the gas diffusion layer or the mixture layer) is divided into two parts, i.e., the water permeation suppressing part closer to the entrance for oxidizer gas and the water permeable part closer to the exit. The layer can be divided into more than two parts arid the water permeability in the three parts can be set to change in stages. Also the water permeability can be set to continuously change from the entrance to the exit, so that the fluororesin content continuously decreases from the entrance to the exit.
Although the present invention has been fully described by way of examples with reference to the accompanying drawings, it is to be noted that various changes and modifications will be apparent to those skilled in the art. Therefore, unless such changes and modifications depart from the scope of the present invention, they should by construed as being included therein. PTFE content in gas diffusion layer on cathode A/B entrance side:A(wt%) exit side;B(wt%) practical example 1 26 25 1.04 practical example 2 30 25 1.20 practical example 3 50 25 2.00 practical example 4 60 25 2.40 comparative example 1 25 25 1.00 comparative example 2 40 40 1.00
entrance side area exit side area carbon specific surface (m2/g) weight ratio of carbon to PTFE carbon specific surface (m2/g) weight ratio of carbon to PTFE practical example 5 100∼150 10:10 700∼800 10 : 10 practical example 6 100∼150 10:10 700∼800 10 : 4.2 practical example 7 100∼150 10:10 200∼300 10 : 10 practical example 8 200∼300 10 :10 700∼800 10 : 10 comparative example 3 200∼300 10 :10 200∼300 10 : 10
entrance side area exit side area weight ratio of carbon to PTFE in mixture layer water repellent content in gas diffusion layer weight ratio of carbon to PTFE in mixture layer water repellent content in gas diffusion layer practical example 9 10 : 10 20wt% 10 : 4.2 20wt% practical example 10 10 : 10 20wt% 10 : 4.2 50wt%
the oxidizer channels that face the cathode catalyst layer, oxidizer passing through the oxidizer channels; and
(D) a water permeability adjusting layer that is disposed on the cathode catalyst layer so as to face the oxidizer channels, the water permeability adjusting layer being conductive and gas-permeable, water permeability of which is set to be lower in an area closer to an entrance for the oxidizer than in an area closer to an exit for the oxidizer.
The fuel cell according to Claim 1, wherein the water permeability adjusting layer is formed by a conductive, porous material that has been processed so that water permeability of the conductive, porous material is lower in a fixed area starting from an end of the water permeability adjusting layer on the side of the entrance for the oxidizer than in a remaining area.
The fuel cell according to Claim 2, wherein the percentage of the fixed area starting from the end of the water permeability adjusting layer on the side of the entrance for the oxidizer to the entire area of the water permeability adjusting layer is 10 to 90.
The fuel cell according to Claim 1, wherein
the content of the water repellent in the area closer to the entrance for the oxidizer is set to be higher than the content of the water repellent in the area closer to the exit for the oxidizer.
The fuel cell according to Claim 4, wherein the content of the water repellent in the water permeability adjusting layer on the side of the entrance for the oxidizer is 1.05 to 2.00 times the content of the water repellent in the water permeability adjusting layer on the side of the exit for the oxidizer.
The fuel cell according to Claim 4, wherein the content of the water repellent to the weight of the water permeability adjusting layer in the area closer to the entrance for the oxidizer is 15 to 90wt%.
The fuel cell according to Claim 4, wherein the water repellent is fluororesin.
the water permeability adjusting layer includes:
the specific surface area of a first carbon material in the area closer to the entrance for the oxidizer is smaller than the Specific surface area of a second carbon material in the area closer to the exit for the oxidizer.
The fuel cell according to Claim 8, wherein the water-repellent material has been added to the carbon material so that water repellency of the mixture layer is higher in the area closer to the entrance for the oxidizer than in the area closer to the exit for the oxidizer.
The fuel cell according to Claim 8, wherein
the specific surface area of the first carbon material is smaller than the specific surface area of the carbon catalyst support in the area closer to the entrance for the oxidizer.
cathode catalyst layer is formed by a carbon catalyst support that supports catalyst, and
the specific surface area of the second carbon material is larger than the specific surface area of the carbon catalyst support in the area closer to the exit for the oxidizer.
The fuel cell according to Claim 12, wherein the content of the water-repellent material to the weight of the mixture layer is no greater than 60w% in the area where the content of the water-repellent material is highest.
The fuel cell according to Claim 12, wherein water repellency of the gas diffusion layer is set to be lower in the area closer to the entrance for the oxidizer than in the area closer to the exit for the oxidizer.
The fuel cell according to Claim 14, wherein
the content of the water-repellent material to the weight of the gas diffusion layer is no greater than 60w% in an area where the content of the water-repellent material is highest.
The fuel cell according to Claim 1, a plurality of the fuel cells being stacked in layers to form a fuel cell stack, the fuel cell stack with channels for coolant between the plurality of the fuel cells, wherein
the coolant and the oxidizer travel in the same direction.
EP00113292A 1999-06-22 2000-06-21 Stable and high-performance fuel cell Expired - Fee Related EP1063717B1 (en)
JP17608499 1999-06-22
JP2000121616 2000-04-21
EP1063717A2 true EP1063717A2 (en) 2000-12-27
EP1063717A3 EP1063717A3 (en) 2004-03-17
EP1063717B1 EP1063717B1 (en) 2011-09-28
EP00113292A Expired - Fee Related EP1063717B1 (en) 1999-06-22 2000-06-21 Stable and high-performance fuel cell
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Inventor name: NAKATO, KUNIHIRO
Inventor name: HAMADA, AKIRA
Inventor name: ISONO, TAKAHIRO
Inventor name: KANEKO, MINORU
Inventor name: MIYAKE, YASUO
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