CN108336382A - It is a kind of using graphene black phosphorus alkene hetero-junctions as hydrogen fuel cell of electrode and preparation method thereof - Google Patents
It is a kind of using graphene black phosphorus alkene hetero-junctions as hydrogen fuel cell of electrode and preparation method thereof Download PDFInfo
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- CN108336382A CN108336382A CN201810020140.3A CN201810020140A CN108336382A CN 108336382 A CN108336382 A CN 108336382A CN 201810020140 A CN201810020140 A CN 201810020140A CN 108336382 A CN108336382 A CN 108336382A
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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
- H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
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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
- H01M8/1007—Fuel cells with solid electrolytes with both reactants being gaseous or vaporised
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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
- H01M2008/1095—Fuel cells with polymeric electrolytes
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Abstract
The invention discloses a kind of using graphene black phosphorus alkene hetero-junctions as hydrogen fuel cell of electrode and preparation method thereof, including anode and cathode, it is connected by proton exchange membrane between anode and cathode, anode includes top electrode, anode graphite alkene layer and anode black phosphorus alkene catalyst layer, cathode includes lower electrode, cathode graphene layer and cathode black phosphorus alkene catalyst layer, anode black phosphorus alkene catalyst layer and cathode black phosphorus alkene catalyst layer are symmetrically mounted on the upper of proton exchange membrane, lower both sides, top electrode is connected to by anode graphite alkene layer on anode black phosphorus alkene catalyst layer, lower electrode is connected to by cathode graphene layer on cathode black phosphorus alkene catalyst layer；The present invention uses Yin/Yang pole main body of the graphene black phosphorus alkene hetero-junctions as hydrogen fuel cell, can improve the efficiency of the fuel cell first step and third step, while the two-dimensional material graphene black phosphorus alkene chosen, hydrogen fuel cell is made very thin；Reduce manufacturing cost.
Description
Technical field
The present invention relates to field of new energy technologies more particularly to a kind of using graphene black phosphorus alkene hetero-junctions as electrode
Hydrogen fuel cell and preparation method thereof.
Background technology
In the 1960s, hydrogen fuel cell has just been applied successfully to space industry.Travel to and fro between space and the earth it
Between " Apollo " airship be just mounted with this device small, capacity is big.Into after the seventies, constantly with people
A variety of advanced hydrogen producing technologies are grasped, quickly, hydrogen fuel cell is just employed for power generation and automobile.Large-scale power station, either water
Electricity, thermoelectricity or nuclear power, are all that the electricity sent out is sent to power grid, user are conveyed to by power grid.But not due to the load of each electricity consumer
Together, power grid is rendered as peak, being then rendered as low ebb sometimes sometimes, this may result in power failure or voltage instability.In addition, traditional fire
The burning capacity of power station about 70% will consume on boiler and steam turbine generator these huge equipment, when burning also
The a large amount of energy can be consumed and discharge a large amount of harmful substance.And generated electricity using hydrogen fuel cell, it is that the chemical energy of fuel is straight
Switch through and be changed to electric energy, need not burn, energy conversion rate up to 60%~80%, and pollute less, noise it is small, device can
Greatly can be small, very flexibly.
2D materials with atomic layer level thickness due to its different from the superior property of body material and by people extensively grind
Study carefully, such as graphene, MoS2Etc..In recent years, another new 2D material lacks layer black phosphorus alkene and can pass through under experimental conditions
The method of mechanical stripping is prepared and receives the extensive concern of people.Black phosphorus is a kind of crystal with metallic luster,
It can be transformed by white phosphorus or red phosphorus, body black phosphorus has direct semiconductor band gap, and shows and the relevant characteristic of the number of plies, few layer
The electron mobility of black phosphorus alkene is 1000cm2/ Vs also has very high leakage current modulation rate so that it is in following nanometer
Application in electronic device has very big potentiality.In addition because it is direct band gap, optical property also has very big compared to other materials
Advantage, be one of the hot spot of current New Two Dimensional investigation of materials.
Current fuel cell is largely hydrogen fuel cell, and the volume of battery is big, and efficiency of combustion is low.Pass through analysis
Learn that the chemical reaction rate at the low mainly negative and positive the two poles of the earth of fuel cell of efficiency is too slow.Volume is primarily due to greatly negative and positive the two poles of the earth
Thickness it is too big.The appearance of two-dimensional material provides new thinking for fuel cell, and graphene has high electron mobility, black
Phosphorus alkene has big surface volume ratio.The negative and positive the two poles of the earth for the fuel cell that the excellent characteristics of the two are bonded can provide higher
Reaction rate.And two-dimensional material is the number of plies that single layer structure can select material requested according to the performance of battery, so that
It is made thin in negative and positive the two poles of the earth of battery, it is final so that the overall volume of battery reaches minimum.
Invention content
In view of the above problems, present invention aims at a kind of reduction manufacturing cost is provided, hydrogen fuel cell is improved
Efficiency the hetero-junctions using two-dimensional material graphene black phosphorus alkene as the cathode of hydrogen fuel cell and anode prepare proton hand over
Change film hydrogen fuel cell and preparation method thereof.
In order to achieve the above object, the technical solution adopted by the present invention is as follows：It is a kind of to utilize graphene black phosphorus alkene hetero-junctions
As the hydrogen fuel cell of electrode, the hydrogen fuel cell includes anode and cathode, is handed over by proton between anode and cathode
It changes film to be connected, the anode includes top electrode, anode graphite alkene layer and anode black phosphorus alkene catalyst layer, the cathode packet
Include lower electrode, cathode graphene layer and cathode black phosphorus alkene catalyst) layer, anode black phosphorus alkene catalyst layer and the catalysis of cathode black phosphorus alkene
Oxidant layer is symmetrically mounted on the upper and lower both sides of proton exchange membrane, and top electrode is connected to anode black phosphorus alkene by anode graphite alkene layer and urges
On agent layer, lower electrode is connected to by cathode graphene layer on cathode black phosphorus alkene catalyst layer.
Graphene black phosphorus alkene of the present invention is heterogeneous to become a kind of stacking formed between black phosphorus alkene layer and graphene
Structure, the connection spacing of graphene layer and black phosphorus alkene catalyst layer is in anode and cathode
The interfloor distance of graphene is in anode graphite alkene layer of the present inventionThe anode black phosphorus alkene catalyst
The interfloor distance of black phosphorus alkene is in layer
Catalyst in the anode black phosphorus alkene catalyst layer of the present invention is Pt, the cathode black phosphorus alkene catalysis
The alloy that catalyst in oxidant layer is Pt and Pb.
It is provided by the invention a kind of using graphene black phosphorus alkene hetero-junctions as the preparation method of the hydrogen fuel cell of electrode,
Preparation method includes the following steps：
1) white phosphorus or red phosphorus are handled at high temperature under high pressure to obtain black phosphorus alkene；
2) the black phosphorus alkene of certain number of plies is obtained using mechanical stripping method, on black phosphorus alkene surface, using chemical vapor deposition one
Graphene black phosphorus alkene hetero-junctions is made in the graphene of given layer number；
3) graphene upper surface evaporates to form platinum metal layer by the emperor himself in graphene black phosphorus alkene hetero-junctions；
4) it uses optical lithographic methods to form the upper electrode metal of fuel cell on platinum metal layer by the emperor himself, evaporates 20nmTi,
20nmPt, 150nmAu；
5) step 2) -4 is repeated) prepare lower electrode；
6) optical lithography and electron-beam vapor deposition method, making is used to form metal connection column.
In the preparation method of the present invention, wherein the detailed preparation method of graphene black phosphorus alkene hetero-junctions is as follows：
(1) white phosphorus is heated to 200-250 DEG C under the air pressure of 1000-1200Pa, obtains sheet black phosphorus；It is shelled by machinery
From method multilayer black phosphorus alkene is separated from black phosphorus crystal；It removes to obtain stratiform black phosphorus alkene by gas ions stripping means again；
(2) black phosphorus block is obtained from the black phosphorus alkene of stratiform, and black phosphorus block is immersed to the solvent of cumyl hydroperoxide CHP
In, then add ultrasonic echography 10-15 minutes；Make its isolated nonwoven fabric from filaments using centrifuge；
(3) black phosphorus alkene film is pulled out from solution using Si substrates, is placed on 50-60 DEG C of warm table and dries, goes except black
Moisture between phosphorus alkene film and Si substrates, while will few layer black phosphorus alkene is stronger is combined with Si substrates；
(4) it obtains containing multilayer black phosphorus alkene structure on black phosphorus alkene Si substrates, under an electron microscope, be removed by probe
Method peels off extra black phosphorus alkene and obtains the black phosphorus alkene of the appropriate number of plies；
(5) the black phosphorus alkene Si substrates obtained in step (4) are put into stove, are continually fed into protective gas and are heated to 1000
DEG C, stop being passed through protective gas after insulation reaction 20min, is passed through carbon-source gas and carries out reaction 30min；After the completion of reaction, close
Carbon-source gas is passed through protective gas and empties carbon-source gas, room temperature is cooled in the environment of protective gas, takes out Si substrates, obtain
Black phosphorus alkene graphene hetero-junctions on to Si substrates；Black phosphorus alkene graphene hetero-junctions on Si substrates is stripped down.
Carbon-source gas of the present invention is methane；Using methane gas directly in the upper surface of black phosphorus alkene using chemical gas
The graphene of certain number of plies is mutually deposited, graphene black phosphorus alkene hetero-junctions is made.
Protective gas of the present invention is hydrogen and argon gas or nitrogen.
The advantage of the invention is that：The present invention uses Yin/Yang pole of the graphene black phosphorus alkene hetero-junctions as hydrogen fuel cell
Main body can improve the efficiency of the fuel cell first step and third step, to improve the efficiency of hydrogen fuel cell, theory meter on the whole
The efficiency of calculation can reach 63%, be higher than the efficiency value 60% of common hydrogen fuel cell under nominal power；It is chosen in the present invention
Two-dimensional material graphene black phosphorus alkene, hydrogen fuel cell can be made very thin, thickness is about the 4/5 of common hydrogen fuel cell；
Due to not using entire platinum as electrode, but use platinum or the absorption modification of platinum metal on black phosphorus alkene surface, this not only may be used
To improve H2And O2Contact of the molecule with metallic atom, moreover it is possible to substantially reduce manufacturing cost.
Description of the drawings
Fig. 1 is the top structure vertical view of black phosphorus alkene graphene hetero-junctions；
Fig. 2 is the Lateral structure schematic diagram of black phosphorus alkene graphene hetero-junctions；
Fig. 3 is the structural schematic diagram of black phosphorus alkene graphene hetero-junctions fuel cell provided by the invention；
Wherein, 1 anode, A top electrodes, B anode graphite alkene layers, C anode black phosphorus alkene catalyst layers, 2 proton exchange membrane, 3 is cloudy
Pole, D cathode black phosphorus alkene catalyst layers, E cathode graphene layers, electrode under F,
Specific implementation mode
The present invention is described in further detail with specific implementation mode for explanation below in conjunction with the accompanying drawings.
Embodiment 1：As shown in Figure 1,2 and 3 is a kind of using graphene black phosphorus alkene hetero-junctions as the hydrogen fuel of electrode electricity
Pond, the hydrogen fuel cell include anode 1 and cathode 3, are connected by proton exchange membrane 2 between anode 1 and cathode 3, institute
The anode 1 stated includes top electrode A, anode graphite alkene layer B and anode black phosphorus alkene catalyst layer C, and the cathode 3 includes lower electrode
F, cathode graphene layer E and cathode black phosphorus alkene catalyst layer D, anode black phosphorus alkene catalyst layer C and cathode black phosphorus alkene catalyst layer D
The upper and lower both sides of proton exchange membrane 2 are symmetrically mounted on, top electrode A is connected to anode black phosphorus alkene by anode graphite alkene layer B and is catalyzed
On oxidant layer C, lower electrode F is connected to by cathode graphene layer E on cathode black phosphorus alkene catalyst layer D.
Wherein.Graphene black phosphorus alkene is heterogeneous to become a kind of stacking provisions formed between black phosphorus alkene layer and graphene, sun
The connection spacing of graphene layer and black phosphorus alkene catalyst layer is in pole and cathodeGraphene in anode graphite alkene layer
Interfloor distance isThe interfloor distance of black phosphorus alkene is in the anode black phosphorus alkene catalyst layerAnode black phosphorus alkene is catalyzed
Catalyst in oxidant layer C is Pt, the alloy that the catalyst in the cathode black phosphorus alkene catalyst layer D is Pt and Pb.
Embodiment 2：As shown in figure 3, provided by the invention a kind of using graphene black phosphorus alkene hetero-junctions as the hydrogen of electrode
The preparation method of fuel cell, includes the following steps：
1) white phosphorus or red phosphorus are handled at high temperature under high pressure to obtain black phosphorus alkene；
2) the black phosphorus alkene of certain number of plies is obtained using mechanical stripping method, on black phosphorus alkene surface, using chemical vapor deposition one
Graphene black phosphorus alkene hetero-junctions is made in the graphene of given layer number；
3) graphene upper surface evaporates to form platinum metal layer by the emperor himself in graphene black phosphorus alkene hetero-junctions；
4) it uses optical lithographic methods to form the upper electrode metal of fuel cell on platinum metal layer by the emperor himself, evaporates 20nmTi,
20nmPt, 150nmAu；
5) step 2) -4 is repeated) prepare lower electrode；
6) optical lithography and electron-beam vapor deposition method, making is used to form metal connection column.
Embodiment 3：As shown in figure 3, in the preparation method of the present invention, the detailed preparation side of graphene black phosphorus alkene hetero-junctions
Method is as follows：
(1) white phosphorus is heated to 200-250 DEG C under the air pressure of 1000-1200Pa, obtains sheet black phosphorus；It is shelled by machinery
From method multilayer black phosphorus alkene is separated from black phosphorus crystal；It removes to obtain stratiform black phosphorus alkene by gas ions stripping means again；
(2) black phosphorus block is obtained from the black phosphorus alkene of stratiform, and black phosphorus block is immersed to the solvent of cumyl hydroperoxide CHP
In, then add ultrasonic echography 10-15 minutes；Make its isolated nonwoven fabric from filaments using centrifuge；
(3) black phosphorus alkene film is pulled out from solution using Si substrates, is placed on 50-60 DEG C of warm table and dries, goes except black
Moisture between phosphorus alkene film and Si substrates, while will few layer black phosphorus alkene is stronger is combined with Si substrates；
(4) it obtains containing multilayer black phosphorus alkene structure on black phosphorus alkene Si substrates, under an electron microscope, be removed by probe
Method peels off extra black phosphorus alkene and obtains the black phosphorus alkene of the appropriate number of plies；
(5) the black phosphorus alkene Si substrates obtained in step (4) are put into stove, are continually fed into nitrogen and are heated to 1000 DEG C, protects
Stop being passed through nitrogen after temperature reaction 20min, is passed through methane and carries out reaction 30min；After the completion of reaction, methane gas is closed, is passed through
Nitrogen empties carbon-source gas, and room temperature is cooled in the environment of nitrogen, takes out Si substrates, obtains the black phosphorus alkene graphite on Si substrates
Alkene hetero-junctions；Black phosphorus alkene graphene hetero-junctions on Si substrates is stripped down.
Embodiment 4：As shown in Figures 2 and 3, of the invention using graphene black phosphorus alkene hetero-junctions as the hydrogen fuel of electrode electricity
The operation principle in pond is as follows：Hydrogen fuel electromagnetism is the principle of the back reaction based on water decomposition, hydrogen and oxygen be supplied respectively to anode and
Cathode, under thermal equilibrium state, graphene black phosphorus alkene hetero-junctions such as Fig. 2.
First, such stacking is that hetero-junctions is most stable of, and the distance between graphene black phosphorus alkene interface isAnd this
Stacking forming process is exothermic process, and it can be 0.141eV/ atoms to be computed its formation, this can provide relatively stable hetero-junctions.
Secondly, graphene part interfloor distance isBlack phosphorus alkene part interfloor distance isSuch structure both can be with
Keep the high mobility of electronics, it is also ensured that catalyst is adequately distributed in interlayer, so as to it is limited be H2Molecule is sent out
Raw reaction is decomposed into H cations and an electronics, and H cations reach cathode by proton exchange membrane, and electronics then passes through graphene
Cathode is reached by electrode again and participates in final step reaction, the O of cathode2In black phosphorus alkene part and H cations and electron reaction shape
Cheng Shui.
Embodiment 5：Due to the use of graphene black phosphorus alkene hetero-junctions as the electrode of hydrogen fuel cell, graphene has well
Electric conductivity, black phosphorus alkene as two-dimensional material there is prodigious surface to be adsorbed with the attachment of Pb alloys for catalyst Pt or Pt, and the two
Adsorption energy be respectively 5.40eV and 2.00eV, adsorption energy big in this way is but also hydrogen fuel cell is operated in quite high temperature
Degree.Also it alleviates due to the use of problem high as electrode cost entire pt.Specific theoretical calculation performance is as follows：
It should be noted that above-mentioned is only presently preferred embodiments of the present invention, protection model not for the purpose of limiting the invention
It encloses, the arbitrary combination made on the basis of the above embodiments or equivalents all belong to the scope of protection of the present invention.
Claims (8)
1. a kind of using graphene black phosphorus alkene hetero-junctions as the hydrogen fuel cell of electrode, the hydrogen fuel cell includes anode
And cathode, which is characterized in that be connected by proton exchange membrane between anode and cathode, the anode includes top electrode, sun
Pole graphene layer and anode black phosphorus alkene catalyst layer, the cathode include lower electrode, cathode graphene layer and cathode black phosphorus alkene
Catalyst layer, anode black phosphorus alkene catalyst layer and cathode black phosphorus alkene catalyst layer are symmetrically mounted on upper and lower the two of proton exchange membrane
Side, top electrode are connected to by anode graphite alkene layer on anode black phosphorus alkene catalyst layer, and lower electrode is connected by cathode graphene layer
It is connected on cathode black phosphorus alkene catalyst layer.
2. as described in claim 1 using graphene black phosphorus alkene hetero-junctions as the hydrogen fuel cell of electrode, which is characterized in that
The graphene black phosphorus alkene is heterogeneous to become a kind of stacking provisions formed between black phosphorus alkene layer and graphene, anode and cathode
The connection spacing of middle graphene layer and black phosphorus alkene catalyst layer is
3. as described in claim 1 using graphene black phosphorus alkene hetero-junctions as the hydrogen fuel cell of electrode, which is characterized in that
The interfloor distance of graphene is in the anode graphite alkene layerBlack phosphorus alkene in the anode black phosphorus alkene catalyst layer
Interfloor distance is
4. as described in claim 1 using graphene black phosphorus alkene hetero-junctions as the hydrogen fuel cell of electrode, which is characterized in that
Catalyst in the anode black phosphorus alkene catalyst layer is Pt, the catalyst in the cathode black phosphorus alkene catalyst layer be Pt with
The alloy of Pb.
5. a kind of as described in claim 1 using graphene black phosphorus alkene hetero-junctions as the preparation side of the hydrogen fuel cell of electrode
Method, which is characterized in that the preparation method includes the following steps：
1) white phosphorus or red phosphorus are handled at high temperature under high pressure to obtain black phosphorus alkene；
2) the black phosphorus alkene of certain number of plies is obtained using mechanical stripping method, on black phosphorus alkene surface, using one given layer of chemical vapor deposition
Graphene black phosphorus alkene hetero-junctions is made in several graphenes；
3) graphene upper surface evaporates to form platinum metal layer by the emperor himself in graphene black phosphorus alkene hetero-junctions；
4) it uses optical lithographic methods to form the upper electrode metal of fuel cell on platinum metal layer by the emperor himself, evaporates 20nmTi, 20nmPt,
150nmAu；
5) step 2) -4 is repeated) prepare lower electrode；
6) optical lithography and electron-beam vapor deposition method, making is used to form metal connection column.
6. it is as claimed in claim 5 using graphene black phosphorus alkene hetero-junctions as the preparation method of the hydrogen fuel cell of electrode,
It is characterized in that, the preparation method of the graphene black phosphorus alkene hetero-junctions is as follows：
(1) white phosphorus is heated to 200-250 DEG C under the air pressure of 1000-1200Pa, obtains sheet black phosphorus；The side of being by mechanically pulling off
Method separates multilayer black phosphorus alkene from black phosphorus crystal；It removes to obtain stratiform black phosphorus alkene by gas ions stripping means again；
(2) black phosphorus block is obtained from the black phosphorus alkene of stratiform, black phosphorus block is immersed in the solvent of cumyl hydroperoxide CHP,
Again plus ultrasonic echography 10-15 minutes；Make its isolated nonwoven fabric from filaments using centrifuge；
(3) black phosphorus alkene film is pulled out from solution using Si substrates, is placed on 50-60 DEG C of warm table and dries, remove black phosphorus alkene
Moisture between film and Si substrates, while will few layer black phosphorus alkene is stronger is combined with Si substrates；
(4) it obtains containing multilayer black phosphorus alkene structure on black phosphorus alkene Si substrates, under an electron microscope, the side removed by probe
Method peels off extra black phosphorus alkene and obtains the black phosphorus alkene of the appropriate number of plies；
(5) the black phosphorus alkene Si substrates obtained in step (4) are put into stove, are continually fed into protective gas and are heated to 1000 DEG C, protects
Stop being passed through protective gas after temperature reaction 20min, is passed through carbon-source gas and carries out reaction 30min；After the completion of reaction, carbon source gas is closed
Body is passed through protective gas and empties carbon-source gas, room temperature is cooled in the environment of protective gas, takes out Si substrates, obtain Si bases
Black phosphorus alkene graphene hetero-junctions on plate；Black phosphorus alkene graphene hetero-junctions on Si substrates is stripped down.
7. it is as claimed in claim 6 using graphene black phosphorus alkene hetero-junctions as the preparation method of the hydrogen fuel cell of electrode,
It is characterized in that, the carbon-source gas is methane.
8. it is as claimed in claim 6 using graphene black phosphorus alkene hetero-junctions as the preparation method of the hydrogen fuel cell of electrode,
It is characterized in that, the protective gas is hydrogen and argon gas or nitrogen.
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| CN113178496A (en) * | 2021-04-28 | 2021-07-27 | 东南大学 | Solar cell based on black phosphorus-like material and preparation method thereof |
| CN113846341A (en) * | 2021-09-18 | 2021-12-28 | 广东工业大学 | Preparation method and preparation device of black phosphorus-graphene heterojunction loaded nickel nitride |
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| CN113846341A (en) * | 2021-09-18 | 2021-12-28 | 广东工业大学 | Preparation method and preparation device of black phosphorus-graphene heterojunction loaded nickel nitride |
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