CN105932313A - Hydrophilic and hydrophobic composite flow field plate for direct methanol fuel cell and preparation method of hydrophilic and hydrophobic composite flow field plate - Google Patents
Hydrophilic and hydrophobic composite flow field plate for direct methanol fuel cell and preparation method of hydrophilic and hydrophobic composite flow field plate Download PDFInfo
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- CN105932313A CN105932313A CN201610410999.6A CN201610410999A CN105932313A CN 105932313 A CN105932313 A CN 105932313A CN 201610410999 A CN201610410999 A CN 201610410999A CN 105932313 A CN105932313 A CN 105932313A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
- H01M8/026—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant characterised by grooves, e.g. their pitch or depth
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/02—Details
- H01M8/0202—Collectors; Separators, e.g. bipolar separators; Interconnectors
- H01M8/0258—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant
- H01M8/0265—Collectors; Separators, e.g. bipolar separators; Interconnectors characterised by the configuration of channels, e.g. by the flow field of the reactant or coolant the reactant or coolant channels having varying cross sections
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1009—Fuel cells with solid electrolytes with one of the reactants being liquid, solid or liquid-charged
- H01M8/1011—Direct alcohol fuel cells [DAFC], e.g. direct methanol fuel cells [DMFC]
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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
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Abstract
The invention discloses a hydrophilic and hydrophobic composite flow field plate for a direct methanol fuel cell. A plurality of two-dimensional divergent type trapezoidal channels are evenly formed in a single side of the hydrophilic and hydrophobic composite flow field plate at intervals; and a hydrophobic layer is arranged on the inner surface of each channel and a hydrophillic layer is arranged on the other surfaces. The invention further provides a preparation method of the hydrophilic and hydrophobic composite flow field plate. The method comprises the steps of: (1) sintering and molding the flow field plate; (2) pretreating the surface of the flow field plate; (3) carrying out a surface deposition technology; (4) carrying out an atmosphere sintering strengthening technology; (5) carrying out a surface modification process; and (6) building a hydrophilic surface. By the hydrophilic and hydrophobic composite flow field plate, an anode product carbon dioxide can be efficiently discharged through the hydrophobic divergent type channels when methanol penetration is effectively hindered by an anode side; the condition of cell performance degradation since the anode product blocks a methanol transmission channel is effectively relieved; and guarantee of fuel supply by the fuel cell under different working current becomes possible, so that the overall performance of the cell is improved.
Description
Technical field
The present invention relates to passive type methanol fuel cell technical field, particularly to a kind of hydrophobe for DMFC compound functional flow field plate and preparation method thereof.
Background technology
DMFC has in electrochemical conversion process by it and need not reform, and energy density is high, and operating environment is gentle, and compact conformation etc. superiority causes the extensive concern of research worker all over the world, put into substantial amounts of research work.General, DMFC can be divided into active and passive direct methanol fuel cell.Active DMFC uses pump and gas compressor to provide methanol fuel and oxygen for battery, and passive direct methanol fuel cell utilizes diffusion and free convection, for battery transport fuel and oxygen.
It is known that, the existence of methanol crossover is the important bottleneck of suppression DMFC development, owing to the methanol that penetrates directly reacts generation mixed potential with the oxygen of negative electrode, methanol crossover inevitably causes the loss of voltage, causes the loss of fuel simultaneously.Before DMFC is really applied in actual life, this problem of methanol crossover must have been resolved.Start with from improving flow field plate structure for these many scholars, flow field plate structure reasonable in design, improves resistance alcohol ability and the discharge capacity of product carbon dioxide.Traditional flow field plate structure has round shape, palisade etc., but this kind of flow-field plate is extremely limited to the raising of resistance alcohol ability, scholar is had to use fiber felt as the resistance alcohol layer of methanol fuel cell, improve the methanol solution optimal concentration of methanol fuel cell, to improving energy content of battery ratio, there is positive role, but, under high current operating conditions, anode produces a large amount of bubbles to be needed to get rid of through fiber felt, this unavoidably blocks the transmission channels of methanol so that methanol hunger phenomenon easily occur at anode, limits the further lifting of methanol fuel cell performance.Can design for this and a realize the flow-field plate that methanol solution and carbon dioxide flows passage be separated from each other and be and important.
Summary of the invention
The shortcoming and defect existed for prior art, the invention discloses a kind of hydrophobe for DMFC compound functional flow field plate and preparation method thereof, hydrophobe compound functional flow field plate is using Porous Cu material-copper powder sintering flat board as matrix, described copper powder sintering flat board by design corresponding punch graphite jig, by sintering directly formation band two-dimensions flaring type trapezoidal conduit.Convection current field plate carries out alkali auxiliary surface oxidation technology and low-surface-energy solution modification process further, reach hydrophobic performance, prevent coming off of super-hydrophobic layer, introduce solid-phase sintering process, enhance the bond strength of superhydrophobic surface structure and matrix, be conducive to its application in passive type liquid and gaseous state DMFC.Further, need to destroy flow-field plate both sides planar hydrophobic Rotating fields, build hydrophilic layer, to this end, use the technique of polishing on sand paper of bearing a heavy burden, quantitatively polish.
The compound functional flow field plate technique scheme of the hydrophobe for DMFC that the present invention provides is as follows:
A kind of hydrophobe for DMFC compound functional flow field plate, it is arranged on the hollow-out parts in the middle of DMFC anode-side collector plate, described hydrophobe compound functional flow field plate one side is evenly spaced apart to have some two-dimensions trapezoidal conduits of flaring type, the inner surface of described conduit is provided with hydrophobic layer, remaining surface is provided with hydrophilic layer, to realize the function of aqueous vapor shunting, described trapezoidal conduit is two-dimensions flaring type, and radial dimension horizontal along conduit is incremented by, to promoting that gas discharge has positive role.
Further, described conduit is the two-dimensions flaring type conduit being gradually increased along flow-field plate width and high direction size.
Further, the cross section of described conduit is isosceles trapezoid.
Further, described hydrophobic layer contact angle is more than 150 °.
Further, the porosity of described hydrophobe compound functional flow field plate is 70% ~ 80%.
The preparation method of functional flow field plate as compound in described hydrophobe, including step:
(1) flow-field plate sinter molding: copper powder and self-control copper scale are uniformly inserted in corresponding graphite jig according to mass ratio 7:3, being incubated two hours sinter moldings in 940 DEG C in being subsequently placed into stove, introducing copper scale does skeleton and prevents flow-field plate sinter molding process significant shrinkage；
(2) flow field plate faces pretreatment: will the heavy burden 20g polishing under 400 mesh sand paper of the flow-field plate that sinter so that two surfacings, and then to immerse alkali cleaning 3 ~ 5min and mass fraction in the NaOH solution that concentration is 150g/L successively be the H of 5wt%2SO4Pickling 3 ~ 5min in solution, finally cleans up with deionized water；
(3) surface depositing operation: the flow-field plate after cleaning is immersed in the deposition solution of surface and deposits 1 ~ 2h, and reaction is taken out after terminating, and air-dries in atmosphere after cleaning up with deionized water；
(4) atmosphere sintering reinforcement process: the flow-field plate after air-drying is put in the atmosphere furnace with protective gas protection, is incubated 1-2h at 300 ~ 500 DEG C；
(5) surface modification processes: the flow-field plate after sinter is immersed in surface and modifies modification 12h ~ 72d in solution, modify and take out after terminating, clean up with acetone reagent, air-dry in then dropping a hint, hydrophobic surface can be obtained in groove；
(6) water-wetted surface is built: polished on 200 mesh sand paper by the flow-field plate heavy burden 10g handled well, polished off by the hydrophobic layer in plane, i.e. can get hydrophobe compound functional flow field plate.
On the one hand, flow-field plate different surfaces hydrophilicity and hydrophobicity is different；On the other hand, groove both ends open is isosceles trapezoid, and to realize double dimension flaring, little mouth down during assembling, big mouth upward, can effectively facilitate the discharge of product.
Process for treating surface is surface depositing operation and surface modification processes, is simultaneously introduced atmosphere sintering reinforcement process, and to strengthen the bond strength of superhydrophobic surface structure and matrix, during preventing from using, super-hydrophobic layer comes off.
Further, deposition solution in described surface is 2mol/L NaOH and 0.2mol/L K2S2O8Deionized water solution.
Further, the stearic acid ethanol solution that solution is 0.01mol/L is modified on described surface.
Further, described protective gas is argon or nitrogen.
Further, described copper powder is 100 mesh atomization dendroid copper powders, and described copper scale is formed by the flat copper billet of milling machine milling.
Compared to existing technology, the invention has the beneficial effects as follows: two-dimensions flaring type flow field conduit can realize liquid edema caused by disorder of QI from, the beneficially discharge of product carbon dioxide.Its reason is that the compound structure of hydrophobe is conducive to separating water flow circulation passage, in strengthening product carbon dioxide is gathered in flaring type conduit and discharge, continuously feeds provide positive direction for realizing methanol.
Accompanying drawing explanation
Fig. 1 hydrophobe compound functional flow field plate schematic diagram.
Fig. 2 hydrophobe compound functional flow field plate and collector plate assembling schematic diagram.
Fig. 3 is the assembling schematic diagram of the DMFC for assembling hydrophobe compound functional flow field plate.
1-negative electrode end cap in figure, 2-cathode collector plate, 3-teflon gasket, 4-silica gel pad, 5-PEM, 6-anode collector plate, 7-anode fuel chamber, 8-conduit.
Detailed description of the invention
Being described in further detail the goal of the invention of the present invention with specific embodiment below in conjunction with the accompanying drawings, embodiment no longer repeats one by one at this, but the most therefore embodiments of the present invention are defined in following example.
Embodiment one
As depicted in figs. 1 and 2, a kind of hydrophobe for DMFC compound functional flow field plate, it is arranged on the hollow-out parts in the middle of DMFC anode-side collector plate 6, described hydrophobe compound functional flow field plate one side is evenly spaced apart to have seven two-dimensions flaring type isosceles conduits 8, described conduit 8 is gradually increased along flow-field plate width with high direction size, and its cross section is isosceles trapezoid.The inner surface of described conduit 8 is provided with hydrophobic layer, and remaining surface is provided with hydrophilic layer.Described hydrophobic layer contact angle is more than 150 °.The porosity of described hydrophobe compound functional flow field plate is 70% ~ 80%, this flow-field plate a size of 30mm × 30mm × 2mm, and its trapezoidal conduit 8 is designed as double dimension flaring type, and seven conduits 8 are distributed on flow-field plate side.
The material of described super hydrophobic porous flow-field plate is atomization dendroid copper powder and self-control copper scale.
As it is shown on figure 3, DMFC is by negative electrode end cap 1 in figure, cathode collector plate 2, teflon gasket 2, silica gel pad 4, PEM 5, anode collector plate 6, anode fuel chamber 7.Described hydrophobe compound functional flow field plate 6 is arranged on the hollow-out parts in the middle of DMFC anode-side collector plate 6, described hydrophobe compound functional flow field plate fluting side is right against DMFC anode-side, to realize high resistance alcohol ability and to realize aqueous vapor channel separation, improve battery stability under different current works.
Hydrophobe compound functional flow field plate can improve the resistance alcohol ability of flow-field plate, the effect of solid steam channel separation simultaneously, thus prevents product carbon dioxide from blocking methanol transmission channels.Concrete operation principle is: methanol passes through to pass fine and close copper powder plate from fuel cavity, owing to copper powder plate space is less, methanol solution spreads slower wherein, thus can realize, directly to battery supplied high concentration methanol solution, improving the energy density of battery in the case of to a certain degree maintaining methanol crossover.On the other hand, anode at DMFC, methanol decomposes generation carbon dioxide under the effect of catalyst, accumulation along with reaction, the air pocket that minute bubbles crossfade into, for conventional flow field plate, bubble will penetrate flow-field plate under the effect of the pressure at membrane electrode, arrive methanol fuel chamber to discharge, and hydrophobe compound functional flow field plate has two-dimensions flaring type conduit 8 due to it in membrane electrode side, bubble spreads toward the place that transmission resistance is little, it is gathered in groove, simultaneously, difference due to hydrophilic and hydrophobic, form a kind of thrust, bubble is pressed in conduit 8 by bubble methanol solution.Bubble is gradually assembled at conduit 8, and buoyancy is gradually increased, simultaneously because the two of conduit 8 flaring type structures so that bubble has component upwards, promotes bubble to pass through conduit 8 further and is discharged to outside battery.Thus avoid under high current density works, produce great amount of carbon dioxide blocking methanol solution transmission channels, to maintaining methanol fuel cell steady operation under different operating electric current, there is positive role.
Embodiment two
The preparation method of a kind of hydrophobe as mentioned compound functional flow field plate, comprises the steps:
Step 1, flow-field plate sinter molding: design flow-field plate trapezoid groove structure and process corresponding punch graphite jig, be incubated 2 hours sinter moldings by HMZ1700-30 vacuum atmosphere electric furnace in 940 DEG C after 4.9952g 100 mesh atomization dendroid copper powder and 2.1408g self-control copper scale are inserted mould；
Step 2, the pretreatment of flow field plate faces: flow-field plate accumulative 1 meter of the heavy burden 20g polishing distance on 400 mesh sand paper that will prepare so that two surfacings, immersing alkali cleaning 240s and mass fraction in the NaOH solution that concentration is 150g/L successively is the H of 5wt%2SO4Pickling 240s in solution, finally cleans up with deionized water；
Step 3, surface depositing operation: the flow-field plate after cleaning is immersed in NaOH that concentration is 2mol/L and concentration is the K of 0.2mol/L2S2O8Deionized water solution in deposit 1.5h, reaction terminate after take out, use deionized water clean up, in air air-dry；
Step 4, atmosphere sintering reinforcement process: the flow-field plate after air-drying is put in the HMZ1700-30 vacuum atmosphere electric furnace with nitrogen protection, be incubated 1.5h at 400 DEG C；
Step 5, surface modification processes: the flow-field plate after step 4 sinter is immersed in the stearic acid ethanol solution that concentration is 0.01mol/L modification 24h, modification is taken out after terminating, use acetone reagent to clean up, then air air-dries, hydrophobic surface can be obtained in groove；
Step 6, structure water-wetted surface: accumulative 0.5 meter of distance of being polished on 200 mesh sand paper by the flow-field plate heavy burden 10g handled well, polish off the hydrophobic layer structure in plane, i.e. can get hydrophobe compound functional flow field plate.
In described step 1, copper scale is formed by the flat copper billet of milling machine milling, and milling machine spindle rotating speed is 2000r/min, and the amount of feeding is 1mm/r, and back engagement of the cutting edge is 0.2mm, and tool diameter is 5mm, after deoxygenation of being deoiled by copper scale after processing.
The above embodiment of the present invention is only for clearly demonstrating example of the present invention, and is not the restriction to embodiments of the present invention.For those of ordinary skill in the field, can also make other changes in different forms on the basis of the above description.Here without also cannot all of embodiment be given exhaustive.All any amendment, equivalent and improvement etc. made within the spirit and principles in the present invention, within should be included in the protection domain of the claims in the present invention.
Claims (10)
1. the hydrophobe compound functional flow field plate for DMFC, it is arranged on the hollow-out parts in the middle of DMFC anode-side collector plate, it is characterized in that: described hydrophobe compound functional flow field plate one side is evenly spaced apart to have some two-dimensions trapezoidal conduits of flaring type, the inner surface of described conduit is provided with hydrophobic layer, and remaining surface is provided with hydrophilic layer.
Hydrophobe the most according to claim 1 compound functional flow field plate, it is characterised in that: described conduit is the two-dimensions flaring type conduit being gradually increased along flow-field plate width and high direction size.
Hydrophobe the most according to claim 1 compound functional flow field plate, it is characterised in that: the cross section of described conduit is isosceles trapezoid.
Hydrophobe the most according to claim 1 compound functional flow field plate, it is characterised in that: described hydrophobic layer contact angle is more than 150 °.
Hydrophobe the most according to claim 1 compound functional flow field plate, it is characterised in that: the porosity of described hydrophobe compound functional flow field plate is 70% ~ 80%.
6. the preparation method of the compound functional flow field of hydrophobe as according to any one of claim 1 to 5 plate, it is characterised in that include step:
(1) flow-field plate sinter molding: copper powder and self-control copper scale are uniformly inserted in corresponding graphite jig according to mass ratio 7:3, is incubated two hours sinter moldings in 940 DEG C in being subsequently placed into stove；
(2) flow field plate faces pretreatment: will the heavy burden 20g polishing under 400 mesh sand paper of the flow-field plate that sinter so that two surfacings, and then to immerse alkali cleaning 3 ~ 5min and mass fraction in the NaOH solution that concentration is 150g/L successively be the H of 5wt%2SO4Pickling 3 ~ 5min in solution, finally cleans up with deionized water；
(3) surface depositing operation: the flow-field plate after cleaning is immersed in the deposition solution of surface and deposits 1 ~ 2h, and reaction is taken out after terminating, and air-dries in atmosphere after cleaning up with deionized water；
(4) atmosphere sintering reinforcement process: the flow-field plate after air-drying is put in the atmosphere furnace with protective gas protection, is incubated 1-2h at 300 ~ 500 DEG C；
(5) surface modification processes: the flow-field plate after sinter is immersed in surface and modifies modification 12h ~ 72d in solution, modify and take out after terminating, clean up with acetone reagent, air-dry in then dropping a hint, hydrophobic surface can be obtained in groove；
(6) water-wetted surface is built: polished on 200 mesh sand paper by the flow-field plate heavy burden 10g handled well, polished off by the hydrophobic layer in plane, i.e. can get hydrophobe compound functional flow field plate.
Preparation method the most according to claim 6, it is characterised in that: described surface deposition solution is 2mol/L NaOH and 0.2mol/L K2S2O8Deionized water solution.
Preparation method the most according to claim 6, it is characterised in that: the stearic acid ethanol solution that solution is 0.01mol/L is modified on described surface.
Preparation method the most according to claim 6, it is characterised in that: described protective gas is argon or nitrogen.
Preparation method the most according to claim 6, it is characterised in that: described copper powder is 100 mesh atomization dendroid copper powders, and described copper scale is formed by the flat copper billet of milling machine milling.
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| CN110957501A (en) * | 2019-12-25 | 2020-04-03 | 华南理工大学 | Double-sided crisscross porous flow field plate for methanol fuel cell and preparation method thereof |
| CN113399231A (en) * | 2021-06-29 | 2021-09-17 | 西南交通大学 | Bionic structured staggered sliding antifriction and wear-resistant surface and preparation method thereof |
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| CN110957501A (en) * | 2019-12-25 | 2020-04-03 | 华南理工大学 | Double-sided crisscross porous flow field plate for methanol fuel cell and preparation method thereof |
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| CN113399231A (en) * | 2021-06-29 | 2021-09-17 | 西南交通大学 | Bionic structured staggered sliding antifriction and wear-resistant surface and preparation method thereof |
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