CN1933221A - Cathode flow field plate for self-breathing micro-proton exchange film fuel cell and producing method - Google Patents
Cathode flow field plate for self-breathing micro-proton exchange film fuel cell and producing method Download PDFInfo
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- CN1933221A CN1933221A CNA2006100304731A CN200610030473A CN1933221A CN 1933221 A CN1933221 A CN 1933221A CN A2006100304731 A CNA2006100304731 A CN A2006100304731A CN 200610030473 A CN200610030473 A CN 200610030473A CN 1933221 A CN1933221 A CN 1933221A
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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- Y02E60/30—Hydrogen technology
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Abstract
This invention relates to a cathode flow field plate structure of a self breathing micro-proton exchange membrane(PEM) fuel battery, in which, said flow field is in a double-layer composite hollow structure, the sizes of which are reduced orderly, namely, the side closing to the air of the flow field plate is processed into a hollow runner vertical to the silicon chip direction and the other side closing to the membrane electrode is processed to a runner vertical to the silicon chip corresponding to the hollow runner closing to the air side to let the silicon chip pass through and the size of each runner closing to the membrane electrode is smaller than that closing to the air.
Description
Technical field
The present invention relates to a kind of cathode flow field plate and manufacture method that self-breathing micro-proton exchange film (PEM) fuel cell is used, belong to the PEM fuel cell field.
Background technology
Fuel cell is the device that a kind of chemical energy with fuel (as hydrogen, methyl alcohol etc.) and oxidant (as oxygen, air etc.) is converted into electric energy.Fuel reacts under the anode catalyst effect and loses electronics, and electronics arrives negative electrode through external circuit, and oxidant obtains electronics at negative electrode and is reduced.For the flow channel of turnover fuel cell being provided for reactant (fuel and oxidant) and product, usually on the pole plate of fuel cell, process the groove of different shape, as point-like groove, snakelike groove and netted groove etc., be called the flow field, corresponding pole plate is called flow-field plate.
In recent years, the fast development along with miniature electronic system, various microsensor, palmtop PC (PDA) and mobile phone etc. has proposed more and more higher requirement to the micro electric source.Proton exchange membrane (PEM) fuel cell is hopeful to satisfy this demand owing to have environmental friendliness, energy conversion efficiency height and higher characteristics such as specific energy, and its microminiaturized research has become focus of domestic and international energy field research.Yet micro fuel cell is not simple " micro " of large-scale fuel cell, can not carry complicated auxiliary system as large-scale fuel cell, this just requires the specific energy advantage of the system that brings into play to greatest extent from the making of structural design and core component.
System oversimplifies in order to make, practicability, people adopt hydrogen or alcohol etc. as anode fuel usually, negative electrode then utilizes diffusion directly to obtain oxygen from air in " breathing certainly " mode and makes oxidant, so be called " self-respiration type " micro-proton exchange-film fuel cell.The negative electrode of these batteries often is processed into engraved structure, makes air can directly be diffused into catalyst surface.The great advantage of self-respiration type micro fuel cell is to have omitted the container that stores oxidant, but simplied system structure not only improve the specific energy of battery, and this battery is more convenient for being installed on the portable type electronic products such as mobile phone and laptop computer.It is 1cm that human Teflon such as Ha S. in 2004 are processed into effective area
2Direct formic acid-air micro-proton exchange-film fuel cell, negative electrode is the hollow out flow field structure that is made of parallel strip groove (long 10mm, wide about 0.1mm), its maximum power density is issued to 18mW/cm at normal temperature, atmospheric pressure
2[Ha S., Adams B., Masel R.I., A miniature air breathing direct formic acid fuel cell[J] .Journal ofPower Sources, 2004,128:119-124].And for example, Schmitz A. etc. utilizes traditional printed-board technology to process plate self-respiration type PEM fuel cell and battery pack, and negative electrode has also adopted parallel bar shaped hollow out electrode plate structure (long 20mm, wide 1.5～4mm does not wait), with pure hydrogen is fuel, and the battery effective area is 10cm
2, maximum power density reaches 110mW/cm
2[A.Schmitz, M.Tranitz, Wager, et al., Planar self-breathing fuel cells[J] .Journal of PowerSources, 2003,118:162-171].
At present, large-scale fuel cell flow field board adopts machining or hot press molding method preparation, material adopts metal, graphite or graphite/polymer composites, and the heavy and bulky shortcoming of quality is all arranged, and is unfavorable for further improving the quality of battery than power and volumetric specific power.Therefore, depend merely on the requirement that conventional method and technology can not satisfy the fuel cell system microminiaturization in most cases.
MEMS (micro electro mechanical system) (MEMS, Micro-Electro-Mechanical Systems) technology has smallness (the little and light weight of volume), accurate machining resolution (less than 1 μ m), machining reproducibility highly, batch operation, integrated and material is selected advantages such as flexible easily, has become the prefered method of processing micro fuel cell at present.MEMS technological break-through limitation of traditional techniques, can make fuel cell body long-pending littler, quality is lighter.Take the lead in using the direct methanol-air self-respiration type fuel battery of MEMS technology preparation as Kelley etc., cathode flow field is to process the column type air flow channel that diameter is 40 μ m on silicon chip, and the effective area of battery is 0.25cm
2[Kelley S C, Deluga G A, Smtr W H.A Miniaturemethanol/air polymer electrolyte fuel cell[J] .Electrochem Solid StateLetters, 2000,3:407-409].Chen Cong and present inventor also once adopted the MEMS technology to prepare miniature point-like hollow out cathode flow field, and cross section of fluid channel is long-pending to be 997 μ m * 997 μ m, battery effective area 1.44cm
2, the maximum power density of battery reaches 110mW/cm under the normal temperature and pressure
2[Chen Cong, Zheng Dan, Zhang Xigui etc.With micro electro mechanical system (MEMS) technology system micro PEMFC and performance study thereof.Power technology, 2006,30 (4): 261-265].
In sum, what the miniature PEM fuel cell cathode flow field of self-respiration type structure adopted basically at present is bar shaped, cylindricality or point-like engraved structure, adopts the battery of this structure all to have the big shortcoming of contact resistance, so battery performance is all not ideal enough.
Summary of the invention
The present invention proposes a kind of cathode flow field plate structure and manufacture method that is applicable to the miniature PEM fuel cell of self-respiration type, described flow-field plate utilizes the MEMS technology to process, and is suitable for the miniature PEM fuel cell of various sizes.
The design feature of described flow-field plate is on thickness is materials such as silicon chip about 300～500 μ m cathode flow field to be processed into the two-layer compound engraved structure, and two-layer hollow out size reduces successively.Promptly process definite shape in a side of flow-field plate, perpendicular to the hollow out runner of silicon chip direction, this side hollow out layer thickness accounts for 40～90% of whole flow-field plate gross thickness, its duty ratio (being the percentage that fretwork area accounts for the battery effective area) 40～90% is as the flow field channel (see figure 1) near air side; Opposite side (promptly near membrane electrode (MEA) side) corresponding above-mentioned hollow out runner place at silicon chip processes the aperture runner perpendicular to silicon chip, silicon chip is run through, each channel size of this side is less than the channel size near air side, this layer thickness accounts for the 10%-60% of whole flow-field plate thickness, duty ratio 40～80% (see figure 2)s.
Described taper is from diminishing to the cross section in the middle of the runner plate near a side surface of air, promptly near the sectional area maximum of the runner on the flow-field plate surface of air one side, and reduces gradually along the thickness direction face of flow-field plate.
Described macropore runner and aperture runner are the combination of equal diameter or taper, that is, the macropore runner is equal diameter shape or taper, and the aperture runner also can be equal diameter or taper, and large and small runner (1) is isodiametric hole; (2) be the hole of taper; (3) top near air one side is isodiametric hole, and bottom is the hole of taper, and opposite side is the multiple situations such as hole of taper.
In a word, the shape of two-layer hollow out runner, size, two layers of thickness and fretwork area account for the percentage of battery effective area to be decided on the requirement of battery.
Described flow-field plate manufacturing process steps:
By the shape and the size in required design two layers flow field plate hole, make photolithography plate; The manufacturing materials of flow-field plate can be selected certain thickness twin polishing monocrystalline silicon disk for use.
(1), forms SiO as etching mask in the silicon chip surface thermal oxidation
2Layer;
(2), form mask graph at silicon chip back side photoetching corrosion window;
(3) carry out the secondary thermal oxidation, form the different SiO of thickness at the silicon chip back side
2Layer copies to thin SiO with the mask graph at the silicon chip back side
2On the layer, and in step (5) as the protective layer at the silicon chip back side;
(4) front alignment photoetching is at the positive mask graph that forms of silicon chip;
(5) adopt dry etching (the deep ion corrosion, DRIE), or dried wet mixing closes etch, or wet etching is at the positive preparation of silicon chip macropore runner, control etching time, thereby the corrosion depth of control runner;
(6) clean the back at BOE solution (6 parts of 40%NH
4F and 1 part of 49%HF mixed solution) in erode the thin one deck SiO in the silicon chip back side
2Thereby, form mask graph at the silicon chip back side;
(7) adopt dry etching (the deep ion corrosion, DRIE), or dried wet mixing closes etch, or wet etching corrodes the aperture runner overleaf, until the silicon substrate break-through;
(8) SiO of removal silicon chip surface remnants
2, can on silicon chip, form the double-deck hollow out flow field structure that designs.
After adopting double-deck hollow out cathode flow field plate of the present invention, improved flow field intensity, can make the oxygen that enters in the battery more even in the membrane electrode surface distributed, improve the effective rate of utilization of catalyst, increasing oxygen contacts with the effective of membrane electrode assembly, reduce the contact resistance of battery, also help the effusion of moisture content, battery performance is significantly improved.(seeing embodiment 1 for details).
Description of drawings
Fig. 1 is the structural representation of flow-field plate provided by the invention near air side.
Fig. 2 is the close MEA side structure schematic diagram of cathode flow field plate of the present invention.
Fig. 3 is the generalized section of flow field structure;
Fig. 4 is the SEM figure of the prepared cathode construction of embodiment 1
(a) photo of close air one side runner; (b) be the photo of the aperture amplification of air side runner back side correspondence
Fig. 5 is be inclined upwardly 30 ° SEM photo of the cross section of Fig. 4 structure
Fig. 6 is the battery schematic diagram that cathode flow field plate provided by the invention is formed
The battery schematic diagram that Fig. 7 forms for the conventional cathode flow-field plate
Fig. 8 is that Fig. 6,7 two kinds of cathode flow field plates are formed relation curve between the current density～power density of batteries and the current density～voltage
Voltage stability comparison when Fig. 9 forms the discharge of battery for double-deck engraved structure of the present invention and individual layer engraved structure.
1 represents pole plate main bodys such as silicon among the figure; 2 is the cell sealing groove; 3 is that flow-field plate is near MEA side and the close corresponding small structure of air side macropore.
Embodiment
Embodiment 1:
Select thickness 350 μ m, resistivity silicon chip less than the N (100) of 15 Ω cm, press structure shown in Fig. 1-3, positive and negative all adopts dry etching (DRIE method) to make the double-deck hollow out flow field structure of negative electrode that effective area is 1.2 * 1.2cm, the air side runner is equal diameter, sectional area 300 * 300 μ m, layer thickness 290 μ m, duty ratio is 70%; Near the membrane electrode side runner also is equal diameter, sectional area 11 μ m * 11 μ m, and duty ratio is 50%, and thickness is 60 μ m.Fig. 4 is the SEM figure of prepared cathode construction, and wherein (a) be the structure photo near air one side runner, (b) be photo (close MEA side) after the small structure of air side runner back side correspondence amplifies; Fig. 5 is be inclined upwardly 30 ° SEM photo of the cross section of this structure; Form one deck conductive layer through physics or chemical method at this flow field micropore surface, stand-by.
With proton exchange membrane (Nafion 1135) successively through 3%～5%H
2O
2(80 ℃) and washed with de-ionized water, 0.5molL
-1H
2SO
4After series of steps such as (80 ℃) are protonated, washed with de-ionized water are handled, get a certain amount of 20%Pt/C catalyst respectively with small amount of deionized water and 1: 1 isopropanol water solution by ultrasonic wave mixing 10min, after dripping mass fraction more successively and be 5% Nafion solution, polytetrafluoroethylene (PTFE) emulsion, continue concussion 10～30min.It is on the carbon paper of 1.2cm * 1.2cm through hydrophobic processing, area that prefabricated catalyst is coated onto 2, carries a platinum amount in the Catalytic Layer and is respectively 0.04mgcm
-2And 0.03mgcm
-2With the above-mentioned carbon paper of Catalytic Layer that scribbles behind 120 ℃ of following vacuumize 12h, place each a slice of both sides of the proton exchange membrane of handling (Nafion 1135) respectively, under 130 ℃, 2～4MPa condition, hot pressing 2min obtains a MEA who is made of hydrogen electrode, air electrode and dielectric film.
Cathode flow field and made membrane electrode (MEA) and anode flow field are formed battery by Fig. 6, with hydrogen is fuel, at 20 ℃, normal pressure, 50%RH, hydrogen flow rate is polarization and the power density curve of measuring battery under the 0.02L/min condition, and it is identical with active area, parallel flow anodic configuration, negative electrode is individual layer hollow out flow field (cross section of fluid channel amasss 997 μ m * 997 μ m), by comparing, the results are shown in Figure 8 with the battery (see figure 7) of quadrat method assembling.The result shows, adopts double-deck hollow out cathode construction of the present invention, makes the battery maximum current density by 0.49A/cm
2(curve b-2 among Fig. 8) is increased to 0.79A/cm
2(curve a-2 among Fig. 8), peak power density is by original 123mW/cm
2(curve b-1 among Fig. 8) is increased to 167mW/cm
2(curve a-1 among Fig. 8), the increase rate of peak power density reaches 35.8%.
With above-mentioned two batteries, at 20 ℃ of normal pressures, 50%RH, hydrogen flow rate measure the constant current discharge characteristic under the 0.02L/min condition, the results are shown in Figure 9.Fig. 9 curve a adopts the battery of negative electrode of the present invention at 200mA/cm
2The constant current discharge characteristic, Fig. 9 curve b is that the battery in monolayer cathodes hollow out flow field is at 140mA/cm
2Constant current discharge characteristic under the condition.As seen, adopt the battery of cathode construction of the present invention, at 200mA/cm
2Voltage is stabilized in about 0.36V during discharge, in addition to be higher than adopt the direct hollow out cathode construction of point-like battery at 140mA/cm
2Stable voltage during discharge (about 0.30V), this result further shows and has adopted cathode construction of the present invention, and battery performance is significantly improved.
Embodiment 2:
Select thickness 350 μ m, resistivity silicon chip less than the N (100) of 15 Ω cm, take and manufacturing process steps (1)-(4) identical method, each is of a size of the corrosion window of 800 μ m * 800 μ m in the positive formation of silicon chip, adopt dry etching (DRIE), the control etching time makes the straight hole that forms isodiametric, dark 250 μ m; Through cleaning, remove the thin one deck SiO in the back side
2After, expose the corrosion window that each is of a size of 100 μ m * 100 μ m, silicon chip is put into 50 ℃, in the KOH solution of 40vol% concentration, the two sides is wet etching simultaneously, until the silicon substrate break-through.Formed two layers flow field structure, top are isodiametric macropore, and bottom is the hole of taper, and top surface area 800 μ m * 800 μ m, following table area are 730 μ m * 730 μ m, macroporous layer thickness 300 μ m, and duty ratio is 80%; The aperture layer is the tapered hole structure, the top surface area 100 μ m * 100 μ m of aperture, and following table area 30 μ m * 30 μ m, bed thickness 50 μ m, duty ratio is 60%.
Embodiment 3:
Select thickness 300 μ m, resistivity silicon chip less than the N (100) of 15 Ω cm, take and manufacturing process steps (1)-(4) identical method, each is of a size of the corrosion window of 1.5mm * 1.5mm in the positive formation of silicon chip, adopt wet etching, promptly at 50 ℃, in the KOH solution of 40vol% concentration, the control etching time makes the bellmouth that forms dark 200 μ m; Through cleaning, remove the thin one deck SiO in the back side
2After, expose the corrosion window that each is of a size of 100 μ m * 100 μ m, silicon chip is put into 50 ℃, the corrosion of 40% (Vol%) KOH solution for continuous is until the silicon substrate break-through.Formed two layers flow field structure, the top surface area of macropore are that 1.5mm * 1.5mm, following table area are the tapered hole of 1.15mm * 1.15mm, macroporous layer gross thickness 250 μ m, and duty ratio is 85%; The aperture layer is the tapered hole structure, aperture top surface area 100 μ m * 100 μ m, and following table area 30 μ m * 30 μ m, bed thickness 50 μ m, duty ratio is 60%.
The invention is not restricted to the foregoing description, anyly be equal to replacement all in protection scope of the present invention of the present invention.
Claims (10)
1, a kind of cathode flow field plate of self-breathing micro-proton exchange film fuel cell is characterized in that described cathode flow field plate is processed into the two-layer compound engraved structure, and two-layer hollow out size reduces successively; Be that flow-field plate is near air one side, be processed into hollow out runner perpendicular to the silicon chip direction, at opposite side near membrane electrode, corresponding near the runner of the hollow out runner place of air side processing perpendicular to silicon chip, silicon chip is run through, and each channel size of close membrane electrode side is less than the channel size near air side.
2, press the cathode flow field plate of the described self-breathing micro-proton exchange film fuel cell of claim 1, it is characterized in that the hollow out layer thickness near air one side accounts for the 40-90% of whole flow-field plate gross thickness, and the percentage that fretwork area accounts for the battery effective area is 40-90%.
3,, it is characterized in that the runner of the flow-field plate of close air one side is the hole of equal diameter shape or the hole of taper by the cathode flow field plate of the described self-breathing micro-proton exchange film fuel cell of claim 1.
4, by the cathode flow field plate of the described self-breathing micro-proton exchange film fuel cell of claim 3, when it is characterized in that described tapered channels, near the sectional area maximum on the surface of the flow-field plate of air one side.
5, press the cathode flow field plate of the described self-breathing micro-proton exchange film fuel cell of claim 1, it is characterized in that the hollow out layer thickness near membrane electrode one side accounts for the 10-60% of whole flow-field plate thickness, and the percentage that fretwork area accounts for the battery effective area is 40-80%.
6,, it is characterized in that the runner of the flow-field plate of close membrane electrode one side is the hole of equal diameter shape or the hole of taper by the cathode flow field plate of the described self-breathing micro-proton exchange film fuel cell of claim 1.
7, press the cathode flow field plate of claim 3 or 6 described self-breathing micro-proton exchange film fuel cells, the shape, the size that it is characterized in that two-layer hollow out runner, two-layer thickness and fretwork area account for the percentage of battery effective area and decide on the requirement of battery.
8, by the cathode flow field plate of claim 3 or 6 described self-breathing micro-proton exchange film fuel cells, it is characterized in that near the hollow out runner of the flow-field plate of air side with near the hollow out runner of electrode film one side being: (1) both sides are isodiametric hole; (2) both sides are tapered hole; (3) top near air one side is isodiametric hole, and bottom is the hole of taper, and opposite side is a tapered hole.
9, the method for the cathode flow field plate of preparation self-breathing micro-proton exchange film fuel cell as claimed in claim 1 is characterized in that processing step is:
(1), forms SiO as etching mask in the silicon chip surface thermal oxidation
2Layer;
(2), form mask graph at silicon chip back side photoetching corrosion window;
(3) carry out the secondary thermal oxidation, form the different SiO of thickness at the silicon chip back side
2Layer copies to thin SiO with the mask graph at the silicon chip back side
2On the layer; And in following step (5) as the protective layer at the silicon chip back side;
(4) front alignment photoetching is at the positive mask graph that forms of silicon chip;
(5) adopt dry etching, wet etching or dried wet mixing to close etch, at the positive preparation of silicon chip macropore runner, control etching time, thereby the corrosion depth of control runner;
(6) clean the back at 6 parts of 40%NH
4Erode the thin one deck SiO in the silicon chip back side in the BOE solution of F and 1 part of 49%HF mixing
2Thereby, form mask graph at the silicon chip back side;
(7) adopt dry etching, wet etching, or dried wet mixing closes etch, corrode the aperture runner overleaf, until the silicon substrate break-through;
(8) SiO of removal silicon chip surface remnants
2, can on silicon chip, form double-deck hollow out flow field structure.
10, press the method for the cathode flow field plate of the described self-breathing micro-proton exchange film fuel cell of claim 9, it is characterized in that dry etching adopts the deep ion corrosion, wet etching adopts the KOH solution of 40vol% concentration.
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| Application Number | Priority Date | Filing Date | Title |
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| CNB2006100304731A CN100397687C (en) | 2006-08-25 | 2006-08-25 | Cathode flow field plate for self-breathing micro-proton exchange film fuel cell and producing method |
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| CN100397687C CN100397687C (en) | 2008-06-25 |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103956509A (en) * | 2014-05-19 | 2014-07-30 | 哈尔滨工业大学 | Ceramic aluminum alloy-based self-breathing alcohol fuel cell |
| CN107039658A (en) * | 2017-03-08 | 2017-08-11 | 同济大学 | A kind of method of low cost batch production metal polar plate |
| CN109148927A (en) * | 2018-09-04 | 2019-01-04 | 重庆大学 | Air-breathing with submergence microjet is without film microfluid fuel cell |
| CN109943846A (en) * | 2017-12-05 | 2019-06-28 | 丰田自动车株式会社 | The manufacturing method of separator for fuel battery |
| CN111276711A (en) * | 2020-05-08 | 2020-06-12 | 天能电池集团股份有限公司 | Air flow channel assembly, fuel cell air cooling stack bipolar plate and preparation method |
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Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO1981000032A1 (en) * | 1979-06-25 | 1981-01-08 | Svenska Utvecklings Ab | Electrochemical cell and gas diffusion electrode for the same |
| CN1305156C (en) * | 2003-09-02 | 2007-03-14 | 中国科学院大连化学物理研究所 | Air self-breathing type micro-direct alcohol fuel cell structure and making method |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN103956509A (en) * | 2014-05-19 | 2014-07-30 | 哈尔滨工业大学 | Ceramic aluminum alloy-based self-breathing alcohol fuel cell |
| CN103956509B (en) * | 2014-05-19 | 2015-11-11 | 哈尔滨工业大学 | Ceramic is Al-alloy based from breathing alcohol fuel cell |
| CN107039658A (en) * | 2017-03-08 | 2017-08-11 | 同济大学 | A kind of method of low cost batch production metal polar plate |
| CN109943846A (en) * | 2017-12-05 | 2019-06-28 | 丰田自动车株式会社 | The manufacturing method of separator for fuel battery |
| CN109148927A (en) * | 2018-09-04 | 2019-01-04 | 重庆大学 | Air-breathing with submergence microjet is without film microfluid fuel cell |
| CN109148927B (en) * | 2018-09-04 | 2021-03-19 | 重庆大学 | Air self-breathing membraneless microfluidic fuel cell with immersed microjets |
| CN111276711A (en) * | 2020-05-08 | 2020-06-12 | 天能电池集团股份有限公司 | Air flow channel assembly, fuel cell air cooling stack bipolar plate and preparation method |
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