CN108336382B - Hydrogen fuel cell using graphene black phosphorus heterojunction as electrode and preparation method thereof - Google Patents

Hydrogen fuel cell using graphene black phosphorus heterojunction as electrode and preparation method thereof Download PDF

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CN108336382B
CN108336382B CN201810020140.3A CN201810020140A CN108336382B CN 108336382 B CN108336382 B CN 108336382B CN 201810020140 A CN201810020140 A CN 201810020140A CN 108336382 B CN108336382 B CN 108336382B
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雷双瑛
孙小龙
陈洁
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    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/10Fuel cells with solid electrolytes
    • H01M8/1004Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/10Fuel cells with solid electrolytes
    • H01M8/1007Fuel cells with solid electrolytes with both reactants being gaseous or vaporised
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00Fuel cells; Manufacture thereof
    • H01M8/10Fuel cells with solid electrolytes
    • H01M2008/1095Fuel cells with polymeric electrolytes
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    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30Hydrogen technology
    • Y02E60/50Fuel cells
    • YGENERAL 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
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Abstract

The invention discloses a hydrogen fuel cell using graphene black phosphorus alkene heterojunction as an electrode and a preparation method thereof, the hydrogen fuel cell comprises an anode and a cathode, the anode and the cathode are connected through a proton exchange membrane, the anode comprises an upper electrode, an anode graphene layer and an anode black phosphorus alkene catalyst layer, the cathode comprises a lower electrode, a cathode graphene layer and a cathode black phosphorus alkene catalyst layer, the anode black phosphorus alkene catalyst layer and the cathode black phosphorus alkene catalyst layer are symmetrically arranged on the upper side and the lower side of the proton exchange membrane, the upper electrode is connected on the anode black phosphorus alkene catalyst layer through the anode graphene layer, and the lower electrode is connected on the cathode black phosphorus alkene catalyst layer through the cathode graphene layer; according to the invention, the graphene black phosphorus alkene heterojunction is used as a cathode/anode main body of the hydrogen fuel cell, so that the efficiency of the first step and the third step of the fuel cell can be improved, and meanwhile, the hydrogen fuel cell is made to be very thin by the selected two-dimensional material graphene black phosphorus alkene; the manufacturing cost is reduced.

Description

Hydrogen fuel cell using graphene black phosphorus heterojunction as electrode and preparation method thereof
Technical Field
The invention relates to the technical field of new energy, in particular to a hydrogen fuel cell using a graphene black phosphorus alkene heterojunction as an electrode and a preparation method thereof.
Background
In the 60's of the 20 th century, hydrogen fuel cells have been successfully used in the aerospace field. The small and large capacity device is installed in the Apollo spacecraft which travels to and from space and earth. After the 70 s, hydrogen fuel cells were soon being used for power generation and automotive applications as people continually master a variety of advanced hydrogen production technologies. Large power stations, whether hydroelectric, thermal or nuclear, send the generated electricity to the grid, which delivers it to the users. However, the load of each power consumer is different, so that the power grid sometimes shows a peak and sometimes shows a valley, which may result in a power failure or unstable voltage. In addition, about 70% of the combustion energy of the conventional thermal power station is consumed by large equipment such as a boiler and a turbine generator, and a large amount of energy and a large amount of harmful substances are also consumed during combustion. The hydrogen fuel cell is used for generating electricity, chemical energy of fuel is directly converted into electric energy, combustion is not needed, the energy conversion rate can reach 60% -80%, pollution is low, noise is low, and the device can be large or small and is very flexible.
2D material with atomic layer thickness due to its differenceThe superior properties of bulk materials have been extensively studied, such as graphene, MoS2And so on. In recent years, another new 2D material, namely, a few-layer black phosphorus alkene, can be prepared by a mechanical stripping method under experimental conditions and is widely noticed. Black phosphorus is a crystal with metallic luster, can be converted from white phosphorus or red phosphorus, has a direct semiconductor band gap and shows the characteristics related to the number of layers, and the electron mobility of few-layer black phosphorus alkene is 1000cm2the/Vs also has very high leakage current modulation rate, so that the application of the/Vs in future nano-electronic devices has great potential. In addition, because the material is a direct band gap, the optical properties of the material have great advantages compared with other materials, and the material is one of the hot spots of the research on the novel two-dimensional material at present.
Most of the current fuel cells are hydrogen fuel cells, which are bulky and have low combustion efficiency. The low efficiency is mainly found by analysis that the chemical reaction rate of the cathode and anode of the fuel cell is too slow. The large volume is mainly caused by the large thickness of the cathode and the anode. The appearance of two-dimensional materials provides a new idea for fuel cells, graphene has high electron mobility, and black phosphorus has a large surface-to-volume ratio. The excellent characteristics of the two can be combined to form the cathode and anode of the fuel cell, which can provide higher reaction rate. And the two-dimensional material is a single-layer structure, the number of layers of the required material can be selected according to the performance of the battery, so that the cathode and the anode of the battery are very thin, and the whole volume of the battery is minimized finally.
Disclosure of Invention
In view of the above problems, the present invention aims to provide a proton exchange membrane hydrogen fuel cell prepared by using a heterojunction of graphene black phosphorus alkene as a cathode and an anode of the hydrogen fuel cell, which reduces the preparation cost and improves the efficiency of the hydrogen fuel cell, and a preparation method thereof.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows: the utility model provides an utilize hydrogen fuel cell of graphite alkene black phosphorus alkene heterojunction as electrode, hydrogen fuel cell include positive pole and negative pole, be connected through proton exchange membrane between positive pole and the negative pole, the positive pole include the upper electrode, positive pole graphite alkene layer and positive pole black phosphorus alkene catalyst layer, the negative pole include bottom electrode, negative pole graphite alkene layer and negative pole black phosphorus alkene catalyst) layer, positive pole black phosphorus alkene catalyst layer and negative pole black phosphorus alkene catalyst layer symmetry install in proton exchange membrane's upper and lower both sides, the upper electrode passes through positive pole graphite alkene layer to be connected on positive pole black phosphorus alkene catalyst layer, the bottom electrode passes through negative pole graphite alkene layer to be connected on negative pole black phosphorus alkene catalyst layer.
The graphene black phosphorus alkene heterojunction is a stacking structure formed between a black phosphorus alkene layer and graphene, and the connection distances between the graphene layer and the black phosphorus alkene catalyst layer in the anode and the cathode are both
Figure BDA0001543290950000021
The interlayer distance of graphene in the anode graphene layer is
Figure BDA0001543290950000023
The distance between the layers of the black phosphorus alkene in the anode black phosphorus alkene catalyst layer is
Figure BDA0001543290950000022
The catalyst in the anode black phosphorus alkene catalyst layer is Pt, and the catalyst in the cathode black phosphorus alkene catalyst layer is an alloy of Pt and Pb.
The invention provides a preparation method of a hydrogen fuel cell by using a graphene black phosphorus alkene heterojunction as an electrode, which comprises the following steps:
1) treating white phosphorus or red phosphorus at high temperature and high pressure to obtain black phosphorus alkene;
2) obtaining a certain number of layers of black phosphorus alkene by adopting a mechanical stripping method, and depositing a certain number of layers of graphene on the surface of the black phosphorus alkene by adopting chemical vapor deposition to obtain a graphene black phosphorus alkene heterojunction;
3) evaporating the upper surface of the graphene in the graphene black phosphorus heterojunction to form a platinum metal layer;
4) forming an upper electrode metal of the fuel cell on the platinum metal layer by photolithography, evaporating 20nmTi, 20nmPt, 150 nmAu;
5) repeating the steps 2) -4) to prepare a lower electrode;
6) and forming the metal wiring terminal by using an optical photoetching and electron beam evaporation method.
In the preparation method, the detailed preparation method of the graphene black phosphorus heterojunction comprises the following steps:
(1) heating white phosphorus to 250 ℃ under the air pressure of 1000-1200Pa to obtain flaky black phosphorus; stripping the multilayer black phosphorus alkene from the black phosphorus crystal by a mechanical stripping method; then stripping by a plasma stripping method to obtain layered black phosphorus alkene;
(2) obtaining a black phosphorus block from layered black phosphorus alkene, immersing the black phosphorus block into a solvent of Cumene Hydroperoxide (CHP), and then performing ultrasonic treatment for 10-15 minutes; separating with centrifuge to obtain layered product;
(3) fishing out the black phosphorus alkene film from the solution by adopting a Si substrate, drying the black phosphorus alkene film on a heating table at 50-60 ℃, removing water between the black phosphorus alkene film and the Si substrate, and simultaneously combining a small layer of black phosphorus alkene with the Si substrate more firmly;
(4) obtaining a multi-layer black phosphorus alkene structure on the black phosphorus alkene Si substrate, and stripping off redundant black phosphorus alkene to obtain a proper number of layers of black phosphorus alkene by a probe stripping method under an electron microscope;
(5) putting the black phosphorus alkene Si substrate obtained in the step (4) into a furnace, continuously introducing protective gas, heating to 1000 ℃, keeping the temperature, reacting for 20min, stopping introducing the protective gas, and introducing carbon source gas for reacting for 30 min; after the reaction is finished, closing the carbon source gas, introducing protective gas to exhaust the carbon source gas, cooling to room temperature in the environment of the protective gas, and taking out the Si substrate to obtain a black phosphorus graphene heterojunction on the Si substrate; and stripping the black phosphorus graphene heterojunction on the Si substrate.
The carbon source gas is methane; and directly depositing a certain number of layers of graphene on the upper surface of the black phosphorus by adopting methane gas through chemical vapor deposition to prepare the graphene black phosphorus heterojunction.
The protective gas is hydrogen and argon or nitrogen.
The invention has the advantages that: according to the invention, the graphene black phosphorus alkene heterojunction is used as the cathode/anode main body of the hydrogen fuel cell, so that the efficiency of the first step and the third step of the fuel cell can be improved, the efficiency of the hydrogen fuel cell is integrally improved, the efficiency of theoretical calculation can reach 63%, and is 60% higher than the efficiency value of a common hydrogen fuel cell under rated power; the two-dimensional material graphene black phosphorus alkene selected in the invention can make the hydrogen fuel cell very thin, and the thickness is about 4/5 of the common hydrogen fuel cell; because the whole platinum is not used as an electrode, platinum or platinum-lead alloy is adsorbed and modified on the surface of the black phosphorus alkene, the H can be improved2And O2The contact between the molecule and the metal atom can greatly reduce the manufacturing cost.
Drawings
Fig. 1 is a top structure plan view of a black graphene heterojunction;
fig. 2 is a schematic side view of a black graphene heterojunction;
fig. 3 is a schematic structural diagram of a black graphene heterojunction fuel cell provided in the present invention;
wherein, 1 anode, A upper electrode, B anode graphene layer, C anode black phosphorus catalyst layer, 2 proton exchange membrane, 3 cathode, D cathode black phosphorus catalyst layer, E cathode graphene layer, F lower electrode,
Detailed Description
The invention is described in further detail below with reference to the following description of the drawings and the detailed description.
Example 1: a hydrogen fuel cell using graphene black graphene heterojunction as an electrode as shown in fig. 1, 2 and 3, the hydrogen fuel cell includes an anode 1 and a cathode 3, the anode 1 and the cathode 3 are connected through a proton exchange membrane 2, the anode 1 includes an upper electrode a, an anode graphene layer B and an anode black graphene catalyst layer C, the cathode 3 includes a lower electrode F, a cathode graphene layer E and a cathode black graphene catalyst layer D, the anode black graphene catalyst layer C and the cathode black graphene catalyst layer D are symmetrically installed on the upper and lower sides of the proton exchange membrane 2, the upper electrode a is connected to the anode black graphene catalyst layer C through the anode graphene layer B, and the lower electrode F is connected to the cathode black graphene catalyst layer D through the cathode graphene layer E.
Wherein. The graphene black phosphorus alkene heterojunction is a stacking structure formed between a black phosphorus alkene layer and graphene, and the connection intervals between the graphene layer and the black phosphorus alkene catalyst layer in the anode and the cathode are both
Figure BDA0001543290950000031
The interlayer distance of graphene in the anode graphene layer is
Figure BDA0001543290950000041
The distance between the layers of the black phosphorus alkene in the anode black phosphorus alkene catalyst layer is
Figure BDA0001543290950000042
The catalyst in the anode black phosphorus alkene catalyst layer C is Pt, and the catalyst in the cathode black phosphorus alkene catalyst layer D is an alloy of Pt and Pb.
Example 2: as shown in fig. 3, the method for preparing a hydrogen fuel cell using a graphene black phosphorus heterojunction as an electrode according to the present invention includes the following steps:
1) treating white phosphorus or red phosphorus at high temperature and high pressure to obtain black phosphorus alkene;
2) obtaining a certain number of layers of black phosphorus alkene by adopting a mechanical stripping method, and depositing a certain number of layers of graphene on the surface of the black phosphorus alkene by adopting chemical vapor deposition to obtain a graphene black phosphorus alkene heterojunction;
3) evaporating the upper surface of the graphene in the graphene black phosphorus heterojunction to form a platinum metal layer;
4) forming an upper electrode metal of the fuel cell on the platinum metal layer by photolithography, evaporating 20nmTi, 20nmPt, 150 nmAu;
5) repeating the steps 2) -4) to prepare a lower electrode;
6) and forming the metal wiring terminal by using an optical photoetching and electron beam evaporation method.
Example 3: as shown in fig. 3, in the preparation method of the present invention, the detailed preparation method of the graphene black phosphorus heterojunction is as follows:
(1) heating white phosphorus to 250 ℃ under the air pressure of 1000-1200Pa to obtain flaky black phosphorus; stripping the multilayer black phosphorus alkene from the black phosphorus crystal by a mechanical stripping method; then stripping by a plasma stripping method to obtain layered black phosphorus alkene;
(2) obtaining a black phosphorus block from layered black phosphorus alkene, immersing the black phosphorus block into a solvent of Cumene Hydroperoxide (CHP), and then performing ultrasonic treatment for 10-15 minutes; separating with centrifuge to obtain layered product;
(3) fishing out the black phosphorus alkene film from the solution by adopting a Si substrate, drying the black phosphorus alkene film on a heating table at 50-60 ℃, removing water between the black phosphorus alkene film and the Si substrate, and simultaneously combining a small layer of black phosphorus alkene with the Si substrate more firmly;
(4) obtaining a multi-layer black phosphorus alkene structure on the black phosphorus alkene Si substrate, and stripping off redundant black phosphorus alkene to obtain a proper number of layers of black phosphorus alkene by a probe stripping method under an electron microscope;
(5) putting the black phosphorus alkene Si substrate obtained in the step (4) into a furnace, continuously introducing nitrogen, heating to 1000 ℃, keeping the temperature, reacting for 20min, stopping introducing nitrogen, and introducing methane for reacting for 30 min; after the reaction is finished, closing methane gas, introducing nitrogen to exhaust carbon source gas, cooling to room temperature in a nitrogen environment, and taking out the Si substrate to obtain a black phosphorus graphene heterojunction on the Si substrate; and stripping the black phosphorus graphene heterojunction on the Si substrate.
Example 4: as shown in fig. 2 and 3, the hydrogen fuel cell using the graphene black phosphorus heterojunction as an electrode according to the present invention operates as follows: the hydrogen fuel electromagnetic is based on the principle of reverse reaction of water decomposition, hydrogen and oxygen are respectively supplied to an anode and a cathode, and under a thermal equilibrium state, a graphene black phosphorus alkene heterojunction is shown in figure 2.
First, the stack is the most heterojunction stable, with the distance between graphene and black phosphorus alkene interfaces being
Figure BDA0001543290950000043
And the process of forming the stack is an exothermic process, the energy of formation of which is calculated0.141 eV/atom, which may provide a more stable heterojunction.
Secondly, the distance between the graphene part layers is
Figure BDA0001543290950000051
The distance between partial black phosphorus alkene layers is
Figure BDA0001543290950000052
Such a structure can maintain high electron mobility and ensure sufficient distribution of the catalyst between the layers, so that the amount of H can be limited2The molecules are reacted and decomposed into H cations and an electron, the H cations reach the cathode through the proton exchange membrane, the electron reaches the cathode through the graphene and the electrode to participate in the last step of reaction, and O of the cathode2The black phospholene moiety reacts with H cations and electrons to form water.
Example 5: the graphene black phosphorus alkene heterojunction is used as an electrode of the hydrogen fuel cell, the graphene has good conductivity, the black phosphorus alkene is used as a two-dimensional material, the large surface is provided for attaching and adsorbing catalyst Pt or Pt and Pb alloy, the adsorption energy of the black phosphorus alkene and the catalyst Pt and Pb alloy is 5.40eV and 2.00eV respectively, and the large adsorption energy enables the hydrogen fuel cell to work at a quite high temperature. The problem of high cost due to the use of the entire pt as electrode is also alleviated. The specific theoretical calculation performance is as follows:
Figure BDA0001543290950000053
it should be noted that the above-mentioned embodiments are merely preferred embodiments of the present invention, and are not intended to limit the scope of the present invention, and any combination or equivalent changes made on the basis of the above-mentioned embodiments are also within the scope of the present invention.

Claims (6)

1. A hydrogen fuel cell using graphene black phosphorus alkene heterojunction as an electrode comprises an anode and a cathode, and is characterized in that the anode is connected with the cathode through a proton exchange membrane, the anode comprises an upper electrode, an anode graphene layer and an anode black phosphorus alkene catalyst layer, the cathode comprises a lower electrode, a cathode graphene layer and a cathode black phosphorus alkene catalyst layer, the anode black phosphorus alkene catalyst layer and the cathode black phosphorus alkene catalyst layer are symmetrically arranged on the upper side and the lower side of the proton exchange membrane, the upper electrode is connected on the anode black phosphorus alkene catalyst layer through the anode graphene layer, and the lower electrode is connected on the cathode black phosphorus alkene catalyst layer through the cathode graphene layer;
the graphene black phosphorus alkene heterojunction is a stacking structure formed between a black phosphorus alkene layer and graphene, and the connection distance between the graphene layer and the black phosphorus alkene catalyst layer in the anode and the cathode is both 3.612A; the interlayer distance of graphene in the anode graphene layer is 5A, and the interlayer distance of black phosphorus in the anode black phosphorus catalyst layer is 15A.
2. The hydrogen fuel cell using the graphene black graphene heterojunction as an electrode according to claim 1, wherein the catalyst in the anode black graphene catalyst layer is Pt, and the catalyst in the cathode black graphene catalyst layer is an alloy of Pt and Pb.
3. A method for manufacturing a hydrogen fuel cell using a graphene black phosphorus heterojunction as an electrode according to claim 1, wherein the method comprises the steps of:
1) heating white phosphorus to 250 ℃ under the air pressure of 1000-1200Pa, and treating to obtain black phosphorus alkene;
2) obtaining a certain number of layers of black phosphorus alkene by adopting a mechanical stripping method, and depositing a certain number of layers of graphene on the surface of the black phosphorus alkene by adopting chemical vapor deposition to obtain a graphene black phosphorus alkene heterojunction;
3) evaporating the upper surface of the graphene in the graphene black phosphorus heterojunction to form a platinum metal layer;
4) forming an upper electrode metal of the fuel cell on the platinum metal layer by photolithography, evaporating 20nmTi, 20nmPt, 150 nmAu;
5) repeating the steps 2) -4) to prepare a lower electrode;
6) and forming the metal wiring terminal by using an optical photoetching and electron beam evaporation method.
4. The method for preparing a hydrogen fuel cell using a graphene black phosphorus heterojunction as an electrode according to claim 3, wherein the method for preparing the graphene black phosphorus heterojunction comprises the following steps:
(1) heating white phosphorus to 250 ℃ under the air pressure of 1000-1200Pa to obtain flaky black phosphorus; stripping the multilayer black phosphorus alkene from the black phosphorus crystal by a mechanical stripping method; then stripping by a plasma stripping method to obtain layered black phosphorus alkene;
(2) obtaining a black phosphorus block from layered black phosphorus alkene, immersing the black phosphorus block into a solvent of Cumene Hydroperoxide (CHP), and then performing ultrasonic treatment for 10-15 minutes; separating with centrifuge to obtain layered product;
(3) fishing out the black phosphorus alkene film from the solution by adopting a Si substrate, drying the black phosphorus alkene film on a heating table at 50-60 ℃, removing water between the black phosphorus alkene film and the Si substrate, and simultaneously combining a small layer of black phosphorus alkene with the Si substrate more firmly;
(4) obtaining a multi-layer black phosphorus alkene structure on the black phosphorus alkene Si substrate, and stripping off redundant black phosphorus alkene to obtain a proper number of layers of black phosphorus alkene by a probe stripping method under an electron microscope;
(5) putting the black phosphorus alkene Si substrate obtained in the step (4) into a furnace, continuously introducing protective gas, heating to 1000 ℃, keeping the temperature, reacting for 20min, stopping introducing the protective gas, and introducing carbon source gas for reacting for 30 min; after the reaction is finished, closing the carbon source gas, introducing protective gas to exhaust the carbon source gas, cooling to room temperature in the environment of the protective gas, and taking out the Si substrate to obtain a black phosphorus graphene heterojunction on the Si substrate; and stripping the black phosphorus graphene heterojunction on the Si substrate.
5. The method of claim 4, wherein the carbon source gas is methane.
6. The method for preparing a hydrogen fuel cell using a graphene black phosphorus heterojunction as an electrode according to claim 4, wherein the shielding gas is hydrogen and argon or hydrogen and nitrogen.
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