CN107146891A - A kind of MEA preparation methods of noble metal catalyst particles distribution gradient - Google Patents
A kind of MEA preparation methods of noble metal catalyst particles distribution gradient Download PDFInfo
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- CN107146891A CN107146891A CN201710326248.0A CN201710326248A CN107146891A CN 107146891 A CN107146891 A CN 107146891A CN 201710326248 A CN201710326248 A CN 201710326248A CN 107146891 A CN107146891 A CN 107146891A
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- noble metal
- metal catalyst
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/88—Processes of manufacture
- H01M4/8825—Methods for deposition of the catalytic active composition
- H01M4/8828—Coating with slurry or ink
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
- H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
- H01M4/926—Metals of platinum group supported on carriers, e.g. powder carriers on carbon or graphite
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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 present invention relates to a kind of MEA preparation methods of noble metal catalyst particles distribution gradient, following steps are specifically included：Cut PEM or carbon paper as needed；The noble metal catalyst particles slurry of various concentrations is prepared, and is sufficiently stirred for；The noble metal catalyst particles slurry of various concentrations is successively coated on PEM or carbon paper, realizes that gradient is distributed noble metal catalyst particles in a thickness direction.Compared with prior art, the present invention advantageously reduces the carrying capacity of noble metal, is conducive to the raising of catalyst utilization, according to oxygen concentration gradients distribution characteristics, the active metal catalyst layer of gradient distribution is built, the consumption of noble metal is reduced, i.e., uses few noble metal in the high place of oxygen concentration, in the place that oxygen concentration is not enough, in order that reduction reaction can fully occur for oxygen, electrochemical reaction is promoted using the noble metal of high content, compared with spraying process, waste is prevented effectively from, cost is reduced.
Description
Technical field
The invention belongs to field of fuel cell technology, and in particular to a kind of noble metal catalyst particles distribution gradient
MEA preparation methods.
Background technology
Proton Exchange Membrane Fuel Cells (hereinafter referred to as fuel cell), is a kind of without Carnot cycle, utilizes fuel (hydrogen
Gas) with the electrochemical reaction of oxidant (typically using air), chemical energy is converted into the TRT of electric energy.By proton
The membrane electrode assembly (MEA) that exchange membrane is constituted with noble metal catalyst is the core component of fuel cell, in the work of fuel cell
During work, membrane electrode needs effectively to open fuel with oxidant barrier, prevents fuel from mixing directization with oxidant
Learn and possibly even set off an explosion under reaction, extreme case, or cell power generation caused by the mutual seepage of fuel and oxidant is imitated
Rate declines the decay with the life-span.
In Proton Exchange Membrane Fuel Cells, anode and cathode Catalytic Layer typically all using carbon-supported nano Pt, Pd noble metal or its
Alloy is used as catalyst.Because using expensive noble metal, as catalyst, the cost that this has resulted in fuel cell is high
Do not occupy, had a strong impact on its commercialization.Moreover, the bullion content in cathode catalysis layer is often 2 to 3 times of anode.This
Be due to oxygen reduction reaction (ORR) it is slower than the oxidation reaction speed of hydrogen, hydrogen is also compared in transmission of the oxygen in Catalytic Layer
Slowly.Therefore, in order to reduce fuel cell cost, it is necessary to improve the utilization rate or activity of noble metal, the loss of noble metal is reduced；
And the anticathode measure of pin can more prove effective.
As shown in Figure 1 during electrochemistry occurs for negative electrode, the oxygen in air is from gas diffusion layers (GDL) to proton
Membrane diffusion is exchanged, and the Hydrogen Proton that anode electrochemical reaction is produced then is transmitted through PEM toward negative electrode.Proton and oxygen
After noble metal catalyst Adsorption meets, occurs ORR reaction generation water, two kinds of reactive materials are withered away.Reaction equation side
Formula is as follows：
Due in cathode catalysis layer, by GDL spread and Lai oxygen concentration and be transmitted to by PEM
Graded is presented in the concentration of proton --- the oxygen concentration obtained by the noble metal of (nearly GDL sides) on the outside of Catalytic Layer compared with
Height, and more past inner side oxygen concentration is lower, the concentration of proton is antithesis.Unbalanced substance reaction concentration is for reacting field
The requirement of the quantity of institute --- noble metal is also inconsistent.In this case, it is dense using traditional, equally distributed active metal
The Catalytic Layer building mode of degree, is unfavorable for reducing the raising of the carrying capacity and utilization rate of noble metal., whereas if according to oxygen
Concentration gradient distribution characteristics, builds the active metal catalyst layer of gradient distribution, can necessarily reduce the consumption of noble metal.I.e. in oxygen
The high place of gas concentration uses few noble metal, and in the not enough place of oxygen concentration, in order that oxygen can fully occur also
Original reaction, then promote electrochemical reaction using the noble metal of high content.In addition, membrane electrode assembly used in fuel cell into
This is higher, if using spraying process, in process of production because the catalyst granules of atomization can fly out effective spraying area, so that
Produce certain waste.
Prepared by membrane electrode assembly, as described in patent CN 200480016800.7, it is possible to resolve noble metal granule concentration distribution is asked
Topic, but ink-jet apparatus deposit catalyst layers are used, because the catalyst granules of atomization can fly out effective spraying area, so as to produce
Certain waste；Such as patent CN03133536.5, Catalytic Layer is divided into double-layer structure, using spraying or doctor blade process, realizes and leads
The concentration ecto-entad gradient of electron ion polymer is incremented by, and the concentration of hydrophober from inside to outside successively decrease by gradient, but does not realize
The gradient distribution of noble metal catalyst particles.
The content of the invention
The purpose of the present invention is exactly to provide a kind of noble metal catalyst particles distribution gradient to solve the above problems
MEA preparation methods, noble metal catalyst particles are directly coated at proton according to the concentration gradient of design in a thickness direction
On exchange membrane or on gas diffusion layers.
The purpose of the present invention is achieved through the following technical solutions：
A kind of MEA preparation methods of noble metal catalyst particles distribution gradient, specifically include following steps：
(1) PEM or carbon paper are cut as needed；
(2) the noble metal catalyst particles slurry of various concentrations is prepared, and is sufficiently stirred for；
(3) the noble metal catalyst particles slurry of various concentrations is successively coated on PEM or carbon paper, realized
The gradient distribution of noble metal catalyst particles in a thickness direction, i.e., up reduced, in gas successively on PEM the bottom of from
Body diffused layer up increases successively the bottom of from.
Further, carried out during the coating of described noble metal catalyst particles slurry using coating machine, the coating machine includes
Coating platform, multiple coating heads for being coated with different slurry concentrations and the hot blast knife for slurry to be dried of vacuum-pumping, tool
Body operating procedure is：
(1) the mobile coating supreme material position of platform, smooth be placed on of ready PEM or carbon paper is coated with platform,
Open vacuum extractor；
(2) rotation coating head makes die lip mouth upward to vertical direction, and injection slurry to whole die lip mouth has slurry to overflow and nothing
Stop during bubble, then coating head is rotated to vertical direction, make die lip mouth down；
(3) according to the thickness of PEM or carbon paper and applies the thickness of Catalytic Layer and set painting grease head highness, according to being applied
Length, width and the thickness setting slurry injection rate of Catalytic Layer, start painting work, coating platform passes through coating head, then through heat
Air knife is heated, and moves to lower material position, then counter motion coating platform passes through other coating head, then is heated through hot blast knife, is so handed over
For being coated.
Further, the bottom plate of described coating platform is metal, duroplasts or carbon, and bottom plate is provided with multiple micropores, micro-
Bore dia is not more than 0.5mm.
Further, described noble metal catalyst particles slurry includes following components and parts by weight content：
Further, described noble metal catalyst is 60wt.%Pt pallium-on-carbon, and described Nafion solution is
5wt.% perfluorinated sulfonic acid solution.
In the present invention, in order to realize that the gradient of noble metal catalyst particles is distributed, using multiple coating heads, difference is injected separately into
Noble metal catalyst particles are directly coated at proton by the noble metal catalyst particles slurry of concentration according to the concentration gradient of design
On exchange membrane or on gas diffusion layers, MEA preparation is realized, advantage is：(1) it is simple to operate, it is only necessary to by the difference of preparation
The slurry of concentration is put into multiple coating heads, you can realize the gradient distribution of noble metal catalyst particles；(2) coating high-efficient, speed
It hurry up, the need for manual operations can meet small lot production, also easily amplify during production in enormous quantities, and realize on this basis certainly
Dynamicization；(3) save, be coated with the counter motion of platform, single coating head works independently, and shortens platform movement length, reduces operation empty
Between, under equal performance, it is prevented effectively from the waste of noble metal and PEM.
The present invention advantageously reduces the carrying capacity of noble metal, is conducive to the raising of catalyst utilization, according to oxygen concentration ladder
Distribution characteristics is spent, the active metal catalyst layer of gradient distribution is built, reduces the consumption of noble metal, i.e., in the high place of oxygen concentration
Using few noble metal, in the place that oxygen concentration is not enough, in order that reduction reaction can fully occur for oxygen, using high content
Noble metal promote electrochemical reaction.Compared with spraying process, the present invention uses slurry knife coating, it is to avoid wastes, reduces cost.
Brief description of the drawings
Fig. 1 is the distribution of noble metal granule concentration gradients and material transitive relation schematic diagram in MEA sections；
Fig. 2 is the MEA polarization curve performance maps that single coating head is prepared with two coating heads；
Fig. 3 is coating machine coating head of the present invention and application place schematic diagram.
Embodiment
The present invention is described in detail with specific embodiment below in conjunction with the accompanying drawings.
Embodiment 1
The present embodiment prepares membrane electrode assembly (MEA) using doctor blade process, and noble metal catalyst particles, which divide two layers, to be coated on
On film, it is coated with using coating machine, coating machine coating head and application place schematic diagram reference picture 3 are comprised the following steps that：
Prepare Catalytic Layer slurry a, by weight 60wt.%Pt/C：5wt.%Monomer solution：Isopropanol：Go from
Sub- water=14：6：38：40 prepare, stirring at normal temperature 1 hour.
Prepare Catalytic Layer slurry b, by weight 60wt.%Pt/C：5wt.%Monomer solution：Isopropanol：Go from
Sub- water=8：3：38：40 prepare stirring at normal temperature 1 hour.
Mobile vacuum is coated with the supreme material position of platform, cuts PEM by certain size, is placed on vacuum platform, opens
Vacuum plant.
Rotating slit extrudes coating head a to vertical direction, and die lip mouth upward, is slowly injected into slurry a, when die lip mouth has slurry equal
Stop injection when even spilling and bubble-free, to ensure in die cavity to be mixed into without air, finally rotate slit extruding coating head to vertical
Direction, die lip mouth down.
Rotating slit extrudes coating head b to vertical direction, and die lip mouth upward, is slowly injected into slurry b, when die lip mouth has slurry equal
Stop injection when even spilling and bubble-free, to ensure in die cavity to be mixed into without air, finally rotate slit extruding coating head to vertical
Direction, die lip mouth down.
Grease head highness is applied according to the thickness of PEM and the thickness setting for applying Catalytic Layer；According to the length of applied Catalytic Layer
Degree, width and thickness setting slurry injection rate, to ensure the continuous free from flaw of coating process.
Start painting work, coating platform first passes through coating head a, then is heated through hot blast knife, moves to lower material position, counter motion
Platform, coating platform passes through coating head b, then is heated through hot blast knife, returns to material position, closes vacuum plant, remove coating, can
Realize the gradient distribution of noble metal catalyst particles in a thickness direction.
The MEA prepared is put on fuel cell platform and evaluated, as a result as shown in Fig. 2 as shown in Figure 2, using
MEA made from two coating heads, its performance is better than using MEA, i.e., noble metal catalyst particles of the present invention made from single coating head
The MEA of gradient distribution has preferably catalytic performance.
The present invention is not limited solely to the embodiment of the above, as long as within the scope of the invention as claimed all by Patent Law
Protection.
Claims (5)
1. a kind of MEA preparation methods of noble metal catalyst particles distribution gradient, it is characterised in that specifically include following step
Suddenly：
(1) PEM or carbon paper are cut as needed；
(2) the noble metal catalyst particles slurry of various concentrations is prepared, and is sufficiently stirred for；
(3) the noble metal catalyst particles slurry of various concentrations is successively coated on PEM or carbon paper, your gold is realized
The gradient distribution of metal catalyst particle in a thickness direction.
2. a kind of MEA preparation methods of noble metal catalyst particles distribution gradient according to claim 1, its feature exists
In described noble metal catalyst particles slurry is carried out when being coated with using coating machine, and the coating machine includes the coating of vacuum-pumping
Platform, multiple coating heads for being coated with different slurry concentrations and the hot blast knife for slurry to be dried, concrete operation step is：
(1) the mobile coating supreme material position of platform, smooth be placed on of ready PEM or carbon paper is coated with platform, opened
Vacuum extractor；
(2) rotation coating head makes die lip mouth upward to vertical direction, and injection slurry to whole die lip mouth has slurry to overflow and bubble-free
When stop, then coating head being rotated to vertical direction, makes die lip mouth down；
(3) according to the thickness of PEM or carbon paper and applies the thickness of Catalytic Layer and set painting grease head highness, according to applying catalysis
Length, width and the thickness setting slurry injection rate of layer, start painting work, coating platform passes through coating head, then through hot blast knife
Heating, moves to lower material position, then counter motion coating platform passes through other coating head, then is heated through hot blast knife, so alternately enters
Row coating.
3. a kind of MEA preparation methods of noble metal catalyst particles distribution gradient according to claim 2, its feature exists
In the bottom plate of described coating platform is metal, duroplasts or carbon, and bottom plate is provided with multiple micropores, and micro-pore diameter is not more than
0.5mm。
4. a kind of MEA preparation methods of noble metal catalyst particles distribution gradient according to claim 1, its feature exists
In described noble metal catalyst particles slurry includes following components and parts by weight content：
5. a kind of MEA preparation methods of noble metal catalyst particles distribution gradient according to claim 4, its feature exists
In the pallium-on-carbon that described noble metal catalyst is 60wt.%Pt, described Nafion solution is molten for 5wt.% perfluorinated sulfonic acid
Liquid.
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| CN201710326248.0A CN107146891B (en) | 2017-05-10 | 2017-05-10 | Preparation method of MEA (membrane electrode assembly) with noble metal catalyst particles distributed in gradient |
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| CN201710326248.0A CN107146891B (en) | 2017-05-10 | 2017-05-10 | Preparation method of MEA (membrane electrode assembly) with noble metal catalyst particles distributed in gradient |
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108365231A (en) * | 2018-02-09 | 2018-08-03 | 上海亮仓能源科技有限公司 | A kind of batch manufacturing method of fuel cell membrane electrode |
| CN108580143A (en) * | 2018-05-22 | 2018-09-28 | 中国第汽车股份有限公司 | A kind of all-solid lithium-ion battery pole plate gradient spraying equipment and spraying method |
| CN110364743A (en) * | 2019-06-17 | 2019-10-22 | 江苏大学 | A kind of dual-catalysis layer structure electrode and preparation method and its application in high temperature membrane cell |
| CN112103543A (en) * | 2020-10-16 | 2020-12-18 | 大连理工大学 | Gradient membrane electrode for proton exchange membrane fuel cell and preparation method thereof |
| WO2021093466A1 (en) * | 2019-11-11 | 2021-05-20 | 上海交通大学 | Cathode catalytic layer structure for enhancing catalyst durability and preparation method therefor |
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| CN205443658U (en) * | 2015-12-24 | 2016-08-10 | 加通汽车内饰(常熟)有限公司 | Small -size coating machine |
| CN106327994A (en) * | 2016-08-18 | 2017-01-11 | 广州市金万正印刷材料有限公司 | Antimicrobial sealing label capable of being torn and stuck for plurality of times and preparation method and application of antimicrobial sealing label |
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| CN1492530A (en) * | 2002-10-24 | 2004-04-28 | 江苏隆源双登电源有限公司 | Process for producing fuel cell film electrode |
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108365231A (en) * | 2018-02-09 | 2018-08-03 | 上海亮仓能源科技有限公司 | A kind of batch manufacturing method of fuel cell membrane electrode |
| CN108365231B (en) * | 2018-02-09 | 2020-04-10 | 河南豫氢动力有限公司 | Batch production method of fuel cell membrane electrode |
| CN108580143A (en) * | 2018-05-22 | 2018-09-28 | 中国第汽车股份有限公司 | A kind of all-solid lithium-ion battery pole plate gradient spraying equipment and spraying method |
| CN110364743A (en) * | 2019-06-17 | 2019-10-22 | 江苏大学 | A kind of dual-catalysis layer structure electrode and preparation method and its application in high temperature membrane cell |
| WO2021093466A1 (en) * | 2019-11-11 | 2021-05-20 | 上海交通大学 | Cathode catalytic layer structure for enhancing catalyst durability and preparation method therefor |
| CN112103543A (en) * | 2020-10-16 | 2020-12-18 | 大连理工大学 | Gradient membrane electrode for proton exchange membrane fuel cell and preparation method thereof |
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| CN107146891B (en) | 2020-06-09 |
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