CN101814616A - Gas diffusion layer for fuel cell and preparation method thereof - Google Patents
Gas diffusion layer for fuel cell and preparation method thereof Download PDFInfo
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- CN101814616A CN101814616A CN201010152857A CN201010152857A CN101814616A CN 101814616 A CN101814616 A CN 101814616A CN 201010152857 A CN201010152857 A CN 201010152857A CN 201010152857 A CN201010152857 A CN 201010152857A CN 101814616 A CN101814616 A CN 101814616A
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- 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
Abstract
The invention discloses a gas diffusion layer for a fuel cell and a preparation method thereof. The gas diffusion layer for the fuel cell at least comprises a porous substrate (1) and a microporous layer (2), wherein the microporous layer is compounded on the surface of the porous substrate close to a catalysis layer. The gas diffusion layer is characterized in that: the porous substrate (1) and the microporous layer (2) are all subjected to lyophobic treatment, and all contain fluoropolymer with the lyophobic function, and the fluoropolymer is only subjected to a one-time sintering process. The gas diffusion layer has the advantages that: 1, the fluoropolymer in the porous substrate and the microporous layer is only subjected to one-time sintering, and is simultaneously sintered, so the fluoropolymer is prevented from being aged due to multiple sintering; and 2, the fluoropolymer in the porous substrate and the microporous layer is subjected to one-time simultaneous sintering, so the bonding force of an interface between the porous substrate and the microporous layer is strengthened.
Description
Technical field
The present invention relates to a kind of gas diffusion layer for fuel cell and preparation method thereof.
Background technology
Fuel cell is efficient with it, pollution is little, reliability is high and plurality of advantages such as easy care, be described as be after waterpower, firepower and nuclear energy the 4th generation Blast Furnace Top Gas Recovery Turbine Unit (TRT).And Proton Exchange Membrane Fuel Cells (PEMFC) is the widest type of fuel cell of adaptability wherein.PEMFC is the at present ripe a kind of technology that hydrogen and airborne oxygen can be combined to clean water and discharge electric energy.Because it uses reproducible energy resources---hydrogen, the reaction of formation thing is a water, has realized zero discharge.
In PEMFC, in order to improve Catalytic Layer and gas diffusion layers (Gas Diffion Layer, GDL) contact performance between, at present, common way is to increase one deck microporous layers (Micro-Porous Layer on porous carbon paper or carbon cloth, MPL), solve the problem that contacts between Catalytic Layer and the gas diffusion layers, for example U.S. Pat 2003/009189, US6733915, US6127059 and Chinese patent 98109696,96198611 grades are thought can effectively solve contact problems between Catalytic Layer and the gas diffusion layers applying uniformly microporous layers that one deck is made up of conductive carbon black and water-repelling agent on the hydrophobic treatment porous substrate.Yet, people's such as Lin result of study shows: along with the washing time of the aqueous water in the fuel cell to MPL and basalis increases, the feasible wherein loss of hydrophobic polymer, thereby what cause carbon dust among the MPL laxly makes contact resistance increase and the ratio of hydrophilic pores increases and produces " waterflooding electrode ", finally makes decline (the Energy ﹠amp of battery performance; Fuel 2008,22,2533-2538).
Therefore, not only needing more needs the hydrophobic technology from GDL is improved by the structure and the failure mechanism of gas diffusion layers (GDL) are studied, and makes that bonding is more stable between the GDL internal material interface.
Summary of the invention
For can improve Proton Exchange Membrane Fuel Cells in long-term high humidity environment Catalytic Layer and gas diffusion layers between contact performance, thereby promote the durability of fuel cell, the invention provides a kind of preparation method of gas diffusion layers.
To achieve these goals, technical scheme of the present invention is: as shown in Figure 2,
A kind of gas diffusion layer for fuel cell which comprises at least porous substrate 1, microporous layers 2, and microporous layers is compounded in the surface of porous substrate near Catalytic Layer one side; The fluoropolymer that all contains hydrophobic function in its porous substrate and the microporous layers, the fluoropolymer that hydrophobic function is arranged that contains in porous substrate and the microporous layers only live through once sintering processes simultaneously.
The preparation method of a kind of gas diffusion layer for fuel cell of the present invention is characterized in that, comprises the steps:
1) preliminary treatment of porous substrate: it is that 5% to 80% fluoropolymer emulsions was placed 5 to 60 minutes that porous substrate is put into mass concentration, at room temperature dries after the taking-up or at 40 ℃ to 200 ℃ following heating, dryings;
2) preparation of microporous layers slip: with carbon black and boiling point is that 80 ℃ to 140 ℃ solvent and mass concentration are that 5% to 80% fluoropolymer emulsions is mixed the back and evenly disperseed, and carbon black and fluoropolymer mass ratio are 1: 0.01～1;
3) microporous layers and porous substrate is compound: adopt to be coated with cream, casting, roll extrusion, spraying, printing or coating process compound with step 2 by lamination under 10 ℃ to 70 ℃ the temperature) the microporous layers slip that obtains is compounded on the pretreated porous substrate of step 1);
4) with the step 3) mesocomplex according to fluoropolymer kind difference wherein, put into 210 ℃ to 400 ℃ scopes and carry out sintering and take out after 5 minutes to 120 minutes, obtain gas diffusion layers.
In the technical scheme of the present invention: described porous substrate is carbon paper, carbon cloth or expanded metal.
Described fluoropolymer emulsions is ptfe emulsion, Kynoar emulsion or perfluoroethylene-propylene emulsion.
Described carbon black is powder, carbon nano-tube or the active carbon micro mist of porous, electrically conductive carbon black, acetylene black.
Described boiling point is that 80 ℃ to 140 ℃ solvent is one or more the mixing in methyl alcohol, ethanol, isopropyl alcohol, propyl alcohol, toluene or the water.Mixing match during arbitrarily two or more mixing is any proportioning.
And traditional repeatedly sintering process generally is earlier at 340 ℃ to 400 ℃ following sintering steps 1) in through pretreated porous substrate, apply the microporous layers slip again, and then sintering processes once, than this traditional through the gas diffusion layers of sintering process preparation repeatedly, the present invention has the following advantages:
1. only experiencing fluoropolymer in the once sintered gas diffusion layers among the present invention has avoided repeatedly causing the aging of polymer behind the sintering;
2. because the fluoropolymer in porous substrate 1 and the microporous layers 2 experiences disposable while sintering, make both interfacial adhesions strengthen.
Description of drawings
Membrane electrode (MEA) schematic diagram of Fig. 1 assembling
Fig. 2 is a gaseous diffusion layer structure schematic diagram of the present invention
Fig. 3 embodiment 1, embodiment 2, and embodiment 3, the battery performance figure of the assembling of embodiment 4 and the prepared gas diffusion layers of comparing embodiment.
Among the figure: 1 porous substrate, 2 microporous layers, 3 Catalytic Layer, 4 proton exchange membrane, 5 catalyst layers, 6 microporous layers, 7 porous substrates.
Embodiment
Embodiment 1:
Ptfe emulsion (mass concentration is 80%) is diluted to 18%, take out after then carbon paper (Toray TGPH-060) being put into the ptfe emulsion 8min that is disposed, in air, hang 10min, put into 100 ℃ baking oven oven dry then and handle 20min, obtain through pretreated carbon paper, standby;
Take by weighing 2g conductive carbon black (granularity 30nm) and be placed in the there-necked flask with 50ml distilled water and stir evenly, measure ptfe emulsion (mass concentration is 60%) 10mL and add in above-mentioned conductive carbon black and the aqueous mixtures and stir 30min, obtain the microporous layers slip, standby;
(area is that 100mm * 200mm) is fixed on the platform of the liquid application system of USI Prism350/450 selectivity with pretreated carbon paper, the amount of loading onto is a 50mL microporous layers slip, machine, be sprayed at carbon paper repeatedly, itself and pretreated carbon paper are combined, spray to all on the pretreated carbon paper until the microporous layers slip; Take off this carbon paper then and be placed in the Muffle furnace, promptly make gas diffusion layers at 350 ℃ of sintering processes 20min.Prepared gas diffusion layers and core component (are loaded with the diaphragm of catalyst, be called for short CCM, present embodiment uses GORE.INC., PRIMEA Series5510 type CCM) be assembled into membrane electrode (MEA) and carry out the monocell performance test, the MEA after the assembling is as shown in Figure 1.With fuel battery test system FCLAB test, the battery testing condition is: the Pt carrying capacity of MEA is 0.4mg/cm
2, the battery testing temperature is 60 ℃, 65 ℃ of the humidification temperature of hydrogen and air, and hydrogen and air pressure are normal pressure, and snake shape gas flowfield, active area are 25cm
2, battery performance is seen accompanying drawing 3.
Embodiment 2:
Ptfe emulsion (mass concentration is 80%) is diluted to 18%, take out after then carbon paper (Toray TGPH-060) being put into the polytetrafluoroethylene (PTFE) emulsion 8min that is disposed, in air, hang 10min, put into 100 ℃ baking oven oven dry then and handle 20min, obtain through pretreated carbon paper, standby;
Take by weighing 2g conductive carbon black (granularity 30nm) and be placed in the there-necked flask with 50ml distilled water and stir evenly, measure ptfe emulsion (concentration is 60%) 10mL and add in above-mentioned carbon black and the aqueous mixtures and stir 30min, obtain the microporous layers slip, standby;
(area is 100mm * 200mm) be fixed on the platform of screen process press (PAD PRINTER ENGCO.LTD.SPP-600FV) with pretreated carbon paper, load onto half tone, the amount of pouring out is a 20mL microporous layers slip, the printing of machining, make the microporous layers slip from silk screen ooze down with hydrophobic treatment after carbon paper combine, can cover uniform one deck on this carbon paper, be printed onto on its carbon paper basically all until the microporous layers slip; Take off carbon paper then and be placed in the Muffle furnace, obtain gas diffusion layers at 400 ℃ of sintering processes 20min.With prepared gas diffusion layers and CCM (GORE.INC., PRIMEASeries5510) assembled battery is tested, the MEA of assembling as shown in Figure 1, with fuel battery test system FCLAB test, the battery testing condition is: the Pt carrying capacity of MEA is 0.4mg/cm
2, the battery testing temperature is 60 ℃, 70 ℃ of the humidification temperature of hydrogen and air, and hydrogen and air pressure are normal pressure, and snake shape gas flowfield, active area are 25cm
2, battery performance is seen accompanying drawing 3.
Kynoar emulsion (mass concentration is 30%) is diluted to 18%, take out after then the fiber non-woven carbon cloth being put into the Kynoar emulsion 8min that is disposed, in air, hang 10min, put into 40 ℃ baking oven oven dry then and handle 20min, obtain through pretreated carbon cloth, standby;
The powder (granularity 30nm) that takes by weighing 20g acetylene black is placed in the there-necked flask with 2000ml distilled water and stirs evenly, and measures Kynoar emulsion (concentration is 30%) 100mL and adds in above-mentioned carbon black and the aqueous mixtures and stir 30min, obtains the microporous layers slip, and is standby;
(area is 100mm * 2000mm) be fixed on the material retractable reel of coating machine (TB-750-12S type) with pretreated fiber non-woven carbon cloth, the amount of pouring out is the charging aperture of 500mL microporous layers slip at coating machine, mix up the cutter distance then, the printing of machining, the microporous layers slip is oozed down and carbon cloth combines from the slit of painting cloth-knife and carbon cloth, can cover uniform one deck microporous layers slip on this preliminary treatment carbon cloth, then through drying in the tunnel cave under 100 ℃; Take off carbon paper then and be placed in the Muffle furnace, obtain gas diffusion layers at 270 ℃ of sintering processes 40min.Prepared gas diffusion layers and CCM (GORE.INC., PRIMEA Series5510) assembled battery are tested, and the MEA of assembling tests with fuel battery test system FCLAB as shown in Figure 1, and the battery testing condition is: the Pt carrying capacity of MEA is 0.4mg/cm
2, the battery testing temperature is 60 ℃, 70 ℃ of the humidification temperature of hydrogen and air, and hydrogen and air pressure are normal pressure, and snake shape gas flowfield, active area are 25cm
2, battery performance is seen accompanying drawing 3.
Embodiment 4
Kynoar emulsion (mass concentration is 30%) is diluted to 18%, take out after then carbon paper (Toray TGPH-060) being put into the Kynoar emulsion 8min that is disposed, in air, hang 10min, put into 40 ℃ baking oven oven dry then and handle 20min, obtain the preliminary treatment carbon paper, standby;
The powder (granularity 30nm) that takes by weighing 2g acetylene black is placed in the there-necked flask with 10ml isopropyl alcohol and 40ml toluene and stirs evenly, measuring Kynoar emulsion (concentration is 40%) 10mL adds in above-mentioned carbon black and isopropyl alcohol and the mixture and stirs 30min, obtain the microporous layers slip, standby;
(area is 100mm * 200mm) be fixed on the platform of screen process press (PAD PRINTER ENG CO.LTD.SPP-600FV) with the preliminary treatment carbon paper, load onto half tone, the amount of pouring out is a 20mL microporous layers slip, the printing of machining, the microporous layers slip is oozed down and the preliminary treatment carbon paper combines from silk screen, can cover uniform one deck on this carbon paper, be printed onto on its carbon paper basically all until the microporous layers slip; Take off carbon paper then and be placed in the Muffle furnace, obtain gas diffusion layers at 210 ℃ of sintering processes 40min.With prepared gas diffusion layers and CCM (GORE.INC., PRIMEASeries5510) assembled battery is tested, the MEA of assembling as shown in Figure 1, with fuel battery test system FCLAB test, the battery testing condition is: the Pt carrying capacity of MEA is 0.4mg/cm
2, the battery testing temperature is 60 ℃, 70 ℃ of the humidification temperature of hydrogen and air, and hydrogen and air pressure are normal pressure, and snake shape gas flowfield, active area are 25cm
2, battery performance is seen accompanying drawing 3.
Comparing embodiment:
Ptfe emulsion (mass concentration is 80%) is diluted to 18%, take out after then carbon paper (Toray TGPH-060) being put into the ptfe emulsion 8min that is disposed, in air, dry 10min, put into 400 ℃ baking oven sintering processes 20min then, obtain the preliminary treatment carbon paper, standby;
Take by weighing 2g conductive carbon black (granularity 30nm) and be placed in the there-necked flask with 50ml distilled water and stir evenly, measure ptfe emulsion (mass concentration is 60%) 10mL and add in above-mentioned carbon black and the aqueous mixtures and stir 30min, obtain the microporous layers slip, standby;
(area is that 100mm * 200mm) is fixed on the platform of the liquid application system of USI Prism350/450 selectivity with the preliminary treatment carbon paper, the amount of loading onto is a 50mL microporous layers slip, machine, spray the preliminary treatment carbon paper repeatedly, itself and this carbon paper is combined, can cover uniform one deck on its carbon paper, spray on the carbon paper all until the microporous layers slip; Taking off carbon paper then is placed in the Muffle furnace at 350 ℃ of sintering processes 20min, with prepared gas diffusion layers and CCM (GORE.INC., PRIMEA Series5510) assembled battery is tested, and the MEA of assembling tests with fuel battery test system FCLAB as shown in Figure 1, the battery testing condition is: the Pt carrying capacity of MEA is 0.4mg/cm2, the battery testing temperature is 60 ℃, 70 ℃ of the humidification temperature of hydrogen and air, and hydrogen and air pressure are normal pressure, snake shape gas flowfield, active area are 25cm
2, battery performance is seen accompanying drawing 3.
Porous substrate shown in the present, water-repelling agent, carbon black, boiling point are 80～120 ℃ solvent, adopt other concrete material of failing to enumerate in different composite method and the example can both realize purpose of the present invention.
Claims (6)
1. a gas diffusion layer for fuel cell is characterized in that, which comprises at least porous substrate (1), microporous layers (2), and microporous layers is compounded in the surface of porous substrate near Catalytic Layer one side; The fluoropolymer that all contains hydrophobic function in its porous substrate and the microporous layers, the fluoropolymer that hydrophobic function is arranged that contains in porous substrate and the microporous layers only live through once sintering processes simultaneously.
2. the preparation method of a gas diffusion layer for fuel cell is characterized in that, comprises the steps:
1) preliminary treatment of porous substrate: it is that 5% to 80% fluoropolymer emulsions was placed 5 to 60 minutes that porous substrate is put into mass concentration, at room temperature dries after the taking-up or at 40 ℃ to 200 ℃ following heating, dryings;
2) preparation of microporous layers slip: with carbon black and boiling point is that 80 ℃ to 140 ℃ solvent and mass concentration are that 5% to 80% fluoropolymer emulsions is mixed the back and evenly disperseed, and carbon black and fluoropolymer mass ratio are 1: 0.01～1;
3) microporous layers and porous substrate is compound: adopt to be coated with cream, casting, roll extrusion, spraying, printing or coating process compound with step 2 by lamination under 10 ℃ to 70 ℃ the temperature) the microporous layers slip that obtains is compounded on the pretreated porous substrate of step 1);
4) with the step 3) mesocomplex according to fluoropolymer kind difference wherein, put into 210 ℃ to 400 ℃ scopes and carry out sintering and take out after 5 minutes to 120 minutes, obtain gas diffusion layers.
3. the preparation method of a kind of gas diffusion layer for fuel cell according to claim 2 is characterized in that, described porous substrate is carbon paper, carbon cloth or expanded metal.
4. the preparation method of a kind of gas diffusion layer for fuel cell according to claim 2 is characterized in that, described fluoropolymer emulsions is ptfe emulsion, Kynoar emulsion or perfluoroethylene-propylene emulsion.
5. the preparation method of a kind of gas diffusion layer for fuel cell according to claim 2 is characterized in that, described carbon black is porous, electrically conductive carbon black, acetylene black powder, carbon nano-tube or active carbon micro mist.
6. the preparation method of a kind of gas diffusion layer for fuel cell according to claim 2 is characterized in that, described boiling point is that 80 ℃ to 140 ℃ solvent is one or more the mixing in methyl alcohol, ethanol, isopropyl alcohol, propyl alcohol, toluene or the water.
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Cited By (11)
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| CN103430365A (en) * | 2011-04-06 | 2013-12-04 | 日产自动车株式会社 | Fuel cell |
| CN104882619A (en) * | 2015-04-30 | 2015-09-02 | 吉林大学 | Field catalyzing controlled fuel cell |
| CN106030879A (en) * | 2014-02-24 | 2016-10-12 | 东丽株式会社 | Gas diffusion electrode substrate |
| CN106104877A (en) * | 2014-03-28 | 2016-11-09 | 东丽株式会社 | Gas-diffusion electrode and manufacture method thereof |
| CN109950593A (en) * | 2019-04-04 | 2019-06-28 | 武汉雄韬氢雄燃料电池科技有限公司 | A kind of fuel cell pack and preparation method thereof based on modularized design |
| CN110556557A (en) * | 2019-09-04 | 2019-12-10 | 珠海格力电器股份有限公司 | Membrane electrode structure and membrane electrode and fuel cell with same |
| CN111169030A (en) * | 2020-02-28 | 2020-05-19 | 成都新柯力化工科技有限公司 | Method for preparing carbon paper for gas diffusion layer of fuel cell by calendering and carbon paper |
| CN111180744A (en) * | 2018-11-09 | 2020-05-19 | 本田技研工业株式会社 | Method for forming gas diffusion layer on carbon paper and carbon paper with gas diffusion layer |
| CN112928296A (en) * | 2019-12-05 | 2021-06-08 | 未势能源科技有限公司 | Membrane electrode assembly and fuel cell stack |
| CN112993280A (en) * | 2021-03-11 | 2021-06-18 | 大连交通大学 | Preparation method of microporous layer of gas diffusion layer of lithium-air battery |
| CN115117407A (en) * | 2021-03-19 | 2022-09-27 | 株式会社斯库林集团 | Membrane electrode assembly with gas diffusion layer and method for producing same |
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| CN103430365A (en) * | 2011-04-06 | 2013-12-04 | 日产自动车株式会社 | Fuel cell |
| CN106030879B (en) * | 2014-02-24 | 2019-06-04 | 东丽株式会社 | Gas diffusion electrode substrate |
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| CN104882619A (en) * | 2015-04-30 | 2015-09-02 | 吉林大学 | Field catalyzing controlled fuel cell |
| CN111180744A (en) * | 2018-11-09 | 2020-05-19 | 本田技研工业株式会社 | Method for forming gas diffusion layer on carbon paper and carbon paper with gas diffusion layer |
| CN109950593A (en) * | 2019-04-04 | 2019-06-28 | 武汉雄韬氢雄燃料电池科技有限公司 | A kind of fuel cell pack and preparation method thereof based on modularized design |
| CN110556557A (en) * | 2019-09-04 | 2019-12-10 | 珠海格力电器股份有限公司 | Membrane electrode structure and membrane electrode and fuel cell with same |
| CN112928296A (en) * | 2019-12-05 | 2021-06-08 | 未势能源科技有限公司 | Membrane electrode assembly and fuel cell stack |
| CN112928296B (en) * | 2019-12-05 | 2022-11-18 | 未势能源科技有限公司 | Membrane electrode assembly and fuel cell stack |
| CN111169030A (en) * | 2020-02-28 | 2020-05-19 | 成都新柯力化工科技有限公司 | Method for preparing carbon paper for gas diffusion layer of fuel cell by calendering and carbon paper |
| CN112993280A (en) * | 2021-03-11 | 2021-06-18 | 大连交通大学 | Preparation method of microporous layer of gas diffusion layer of lithium-air battery |
| CN112993280B (en) * | 2021-03-11 | 2023-11-14 | 大连交通大学 | Preparation method of microporous layer of gas diffusion layer of lithium air battery |
| CN115117407A (en) * | 2021-03-19 | 2022-09-27 | 株式会社斯库林集团 | Membrane electrode assembly with gas diffusion layer and method for producing same |
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Application publication date: 20100825 |