CN114708934A - Design method for changing conductivity of graphene and metal interface through stress - Google Patents
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 120
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 119
- 229910052751 metal Inorganic materials 0.000 title claims abstract description 111
- 239000002184 metal Substances 0.000 title claims abstract description 107
- 238000000034 method Methods 0.000 title claims abstract description 43
- 238000013461 design Methods 0.000 title claims abstract description 20
- 239000002131 composite material Substances 0.000 claims abstract description 18
- 239000002905 metal composite material Substances 0.000 claims abstract description 16
- 239000011159 matrix material Substances 0.000 claims abstract description 8
- 230000006835 compression Effects 0.000 claims abstract description 6
- 238000007906 compression Methods 0.000 claims abstract description 6
- 230000001105 regulatory effect Effects 0.000 claims abstract description 5
- 239000010949 copper Substances 0.000 claims description 45
- 239000000463 material Substances 0.000 claims description 17
- 239000010953 base metal Substances 0.000 claims description 16
- 238000004088 simulation Methods 0.000 claims description 11
- 229910052802 copper Inorganic materials 0.000 claims description 8
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 7
- 238000003775 Density Functional Theory Methods 0.000 claims description 7
- 238000004613 tight binding model Methods 0.000 claims description 6
- 229910052782 aluminium Inorganic materials 0.000 claims description 3
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 3
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 2
- 230000001276 controlling effect Effects 0.000 claims description 2
- 229910052749 magnesium Inorganic materials 0.000 claims description 2
- 239000011777 magnesium Substances 0.000 claims description 2
- 238000012216 screening Methods 0.000 claims description 2
- 238000002474 experimental method Methods 0.000 description 8
- 125000004429 atom Chemical group 0.000 description 5
- 238000004364 calculation method Methods 0.000 description 4
- 238000010586 diagram Methods 0.000 description 4
- 239000000758 substrate Substances 0.000 description 3
- 125000004432 carbon atom Chemical group C* 0.000 description 2
- 230000005610 quantum mechanics Effects 0.000 description 2
- 238000011160 research Methods 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
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- 238000011161 development Methods 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- 238000011156 evaluation Methods 0.000 description 1
- 239000007769 metal material Substances 0.000 description 1
- 239000011156 metal matrix composite Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
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Abstract
The invention discloses a design method for changing the conductivity of a graphene and metal interface through stress, and belongs to the technical field of composite materials. The method comprises (1) calculating lattice parameters of graphene and a metal matrix; (2) constructing a metal/graphene/metal composite interface model; (3) determining the appearance of a stably combined metal/graphene/metal interface; (4) modeling and calculating a theoretical conductance value of the interface model; (5) calculating and simulating the conductance value of the metal/graphene/metal interface model under different tension and compression conditions, and evaluating the influence of stress strain on the conductivity of the composite interface; (6) the conductivity of the interface of the graphene/metal composite material is regulated and controlled by applying different stresses. The method can regulate and control the conductivity of the graphene/metal composite material interface by applying stress theoretically, can simply and quickly evaluate the influence of stress strain on the conductivity of the graphene/metal interface by the method, and has important theoretical and practical values.
Description
Technical Field
The invention relates to a theoretical design method for changing the conductivity of a graphene and metal interface through stress, which can be used for predicting the conductivity of the composite material interface, particularly predicting the conductivity of the graphene/metal composite material interface and belongs to the technical field of composite materials.
Background
The graphene material with high strength and high in-plane conductivity is combined with traditional metals such as copper and aluminum to improve the mechanical and electrical properties of the whole material, and is an important research hotspot in the field of graphene reinforced metal matrix composite materials in recent years. The graphene has high-quality conductivity up to 107S·m-1And the material has great potential as a reinforcing phase, so that the material is widely applied to composite materials. When the graphene is combined with the metal substrate, although the thickness of the graphene is very thin compared with that of the metal substrate, electrons still scatter through an interface, so that the improvement of the electrical property of the composite material is restricted, and the conductive efficiency of the graphene reinforced material is not obvious enough. The interface conductance between graphene and a metal material is of great importance in the electrical application of the composite material, but the interface conductance between the atomic-scale two-dimensional material and the base metal is characterized by certain difficulty in experiments, and the experiments have the problems of high equipment requirement, high price and the like, and a large amount of manpower and material resources are needed, so that the quantitative description of the graphene/metal interface conductance and the reasonable design of a local interface atomic structure are hindered.
In order to adapt to different experimental conditions and meet the requirement of service performance, the test work of the conductivity is increased mainly by adopting a frequent trial and error mode in the experiment, and the method is long in time consumption, high in labor consumption and high in cost. With the development of modern theories and computer technologies, the computational thermodynamics, the kinetic simulation and the standard evaluation experiment data are comprehensively utilized in the computational materials science to predict a numerical model, so that the experiment period can be greatly shortened. The simulation process can be completed only on a computer, is basically not limited by experimental conditions, time and space, has extremely strong flexibility and randomness, and is widely applied to the field of composite material design. The first principle calculation method in the computational materials science can not only analyze the influence of stress on the interface conductance from the atomic layer surface, but also can even comprehensively and deeply research the interface conduction behavior and regulate and control the interface conduction performance from the theoretical angle.
Therefore, it is of great significance to design a theoretical design method for changing the conductivity of the interface between graphene and metal through stress.
Disclosure of Invention
The invention aims to provide a method for predicting the interface conductivity of a graphene/metal composite material, and the method can be used for simply and quickly evaluating the influence of stress strain on the interface conductivity of the graphene/metal composite material so as to reduce the complexity and cost of experimental operation and shorten the experimental period, and has important theoretical and practical values.
In order to achieve the purpose, the invention adopts the following technical scheme:
a design method for changing the conductivity of a graphene and metal interface through stress comprises the following steps:
(1) calculating the lattice parameters of the graphene and the base metal: obtaining lattice constants of graphene and base metal by a first principle method of quantum mechanics in computational materials science;
(2) constructing a metal/graphene/metal composite interface model: the matrix metal is used as a main body, a metal/graphene/metal interface model is constructed by utilizing the lattice parameter of the metal, and the method adoptsThe graphene expansion surface;
(3) determining the morphology of the stably bonded metal/graphene/metal interface: graphene as an intermediate layer can generate relative slippage, and the stably combined metal/graphene/metal interface morphology is determined by calculating the interface combination energy of the graphene and the matrix metal;
(4) and (3) modeling and calculating theoretical conductance values of the interface model: performing device modeling on the stably combined composite interface by an unbalanced Green function method based on a density functional theory and simulating and calculating a conductance value of the interface;
(5) calculating and simulating the conductance value of the metal/graphene/metal interface model under different tension and compression conditions to obtain a relation curve graph of stress strain and the conductivity of the composite interface;
(6) and regulating and controlling the conductivity of the graphene/metal composite material interface by applying different stresses according to a strain-conductivity curve graph.
The base metal can be copper, aluminum, magnesium and the like; and repeating the steps aiming at different metal elements to obtain a strain-conductance curve graph.
In the step (2), when a metal/graphene/metal composite interface model is constructed, the thickness of the base metal layer is at least 12 atoms; the base metal surface orientation is determined by simulation or experimental results.
In the step (3), the shape of a stably combined metal/graphene/metal interface is preferentially determined through relative sliding operation, and then the conductance value of the interface is calculated by an unbalanced Green function method based on a density functional theory. The sliding behavior of graphene between metal layers directly influences the appearance of an interface and influences the conductivity of the interface.
In the design method, the stably combined metal/graphene/metal interface morphology is determined by taking the influence of the stably combined metal/graphene/metal interface morphology on a high interface binding energy value as a judgment basis, constructing models aiming at different interface morphologies and calculating the interface binding energy, and screening the stably combined metal/graphene/metal interface morphology.
In the step (5), a relation curve of the strain and the metal/graphene/metal interface conductivity value is obtained through quantum mechanical first-nature principle simulation, and the influence of the applied stress strain on the adjustment of the composite interface conductivity is theoretically evaluated.
The invention has the advantages that:
the invention provides a theoretical design method for changing the conductivity of a graphene and metal interface through stress, the method can be used for reasonably and effectively researching the influence of stress strain on the conductivity of the graphene/metal interface, and the method is more detailed and deeper and has very wide application value. The method greatly reduces the expenditure of manpower and material resources in the traditional experimental method by means of computational materials science.
Drawings
Fig. 1 is a schematic diagram of the Cu (111)/graphene/Cu (111) interface structure in example 1.
Fig. 2 is a schematic structural diagram (front view) of a device of Cu (111)/graphene/Cu (111) in example 1.
Fig. 3 is a side view of the device architecture of Cu (111)/graphene/Cu (111) in example 1.
FIG. 4 is a graph of stress strain versus interface conductance.
The invention is illustrated in detail below by means of the figures and examples, without however implying any limitation to the scope of protection of the invention.
Detailed Description
The invention discloses a theoretical design method for changing the conductivity of a graphene and metal interface through stress, which comprises the following steps:
(1) calculating the lattice parameters of the graphene and the base metal: the lattice constants of the graphene and the base metal are obtained by a quantum mechanical first principle method in the computational materials science.
(2) Constructing a metal/graphene/metal composite interface model: considering a metal substrate as a main body, constructing a metal/graphene/metal interface model by using the lattice parameters of metal, and adoptingWhen the graphene expansion surface is constructed, the thickness of the base metal layer is at least 12 layers of atoms, and the surface orientation is determined by simulation or experimental results.
(3) Determining the morphology of the stably bonded metal/graphene/metal interface: considering that relative slippage can be generated when graphene is used as an intermediate layer, the stably-combined metal/graphene/metal interface morphology is determined by calculating the interface combination energy of the graphene and a metal matrix, and the slippage behavior of the graphene between metal layers directly influences the interface morphology and influences the conductivity of an interface. The stably combined metal/graphene/metal interface morphology is determined mainly by taking the influence of the stably combined metal/graphene/metal interface morphology on a high interface binding energy value as a judgment basis, a model is constructed for different interface morphologies, the interface binding energy is calculated, and finally the stably combined metal/graphene/metal interface morphology can be screened out.
(4) And (3) modeling and calculating theoretical conductance values of the interface model: and (3) performing device modeling on the stably combined composite interface and simulating and calculating the conductance value of the interface by an unbalanced Green function method based on a density functional theory.
(5) Calculating and simulating the conductance value of a metal/graphene/metal interface model under different tension and compression conditions, and evaluating the influence of stress strain on the conductivity of the composite interface: a relation curve of strain and metal/graphene/metal interface conductivity value is obtained through quantum mechanics first-nature principle simulation, and the influence of applied stress strain on the adjustment of the conductivity of the composite interface is theoretically evaluated.
(6) And repeating the steps for different metal elements to obtain a strain-conductance curve graph.
And according to the obtained strain-conductance curve diagram, obtaining the required graphene and metal interface conductivity by selecting proper stress strain.
Taking the base metal copper as an example, the implementation steps of the invention comprise: firstly, calculating lattice parameters of graphene and metal copper, then constructing a metal/graphene/metal composite interface model, considering the influence of relative slippage of graphene as an intermediate layer, determining the shape of a stably combined metal/graphene/metal interface by a computational materials method or an experimental result, modeling to calculate a theoretical conductance value of the interface model, finally calculating and simulating the conductance value of the metal/graphene/metal interface model under different tension and compression conditions, and evaluating the influence of stress strain on the conductivity of the composite interface.
Example 1
Taking a Cu (111)/graphene/Cu (111) interface as an example, the theoretical design method for changing the conductivity of the graphene and metal interface through stress comprises the following steps:
1. calculating the lattice constants of graphene and metallic Cu: the lattice constants of the graphene and the base metal are obtained by a quantum mechanical first principle method in computational materials science, and the lattice constant of the graphene can be obtained to beThe lattice constant of Cu is
2. Constructing a Cu (111)/graphene/Cu (111) interface: as the experiment mostly adopts the growth of graphene on the Cu (111) surface, the invention directly adopts the Cu (111) surface and the Cu (111) surface for the simulation of the graphene/copper interfaceThe surface of the graphene is expanded, the number of metal atoms is 12, and the surface orientation is determined by simulation or experimental results. Fig. 1 is a schematic structural diagram of a Cu (111)/graphene/Cu (111) interface model, and a front view and a side view are respectively shown in fig. 2 and fig. 3, where a large black sphere is a Cu atom and a small black sphere is a C atom.
3. Determining the stably combined Cu (111)/graphene/Cu (111) interface morphology: considering that relative slip is generated when graphene is used as an intermediate layer, the stably-combined Cu (111)/graphene/Cu (111) interface morphology is determined by calculating the interface combination energy of the graphene and a metal matrix, and the slip behavior of the graphene between metal layers directly influences the interface morphology and influences the conductivity of the interface. The formula of the interfacial bonding energy of the graphene and the Cu matrix is as follows:
wherein EtotalAs the total energy of the whole interface system,is the energy of the copper simple substance in the reference state,is the carbon elemental energy, N, of graphene in a reference stateCuAnd NCRespectively the number of Cu atoms and C atoms in the system, and the simulation calculation result shows that the Cu (111)/graphene/Cu (111) boundaryBinding energy E most stable for surface bindingbIs-3.002 eV, and the most stable structure is the top-fcc configuration.
4. And (3) modeling and calculating theoretical conductance values of the interface model: the stably combined Cu (111)/graphene/Cu (111) interface model is converted into an open type double-electrode device system as shown in fig. 2 and 3, the system is divided into a left electrode, a central scattering area and a right electrode, and the transport direction z is from the left electrode to the right electrode. Fig. 2 is a front view and fig. 3 is a side view of a device system of Cu (111)/graphene/Cu (111). Quantum transport calculation is carried out by using an unbalanced Green function method based on a density functional theory to obtain the transport property of an interface system, and a total conductance calculation formula is as follows:
G=(2e2/h)T
where e is the electron charge, h is the planck constant, and T is the transmission coefficient, which can be obtained by solving the green's function of the central scattering region. Dividing the total conductance G by the cross-sectional area as shown in fig. 2-2 yields the total conductance per unit area.
(5) Calculating and simulating the conductance values of the metal/graphene/metal interface model under different tensile and compression conditions: stretching or compressing a Cu (111)/graphene/Cu (111) interface model by 1% along the z-axis direction, repeating the steps, obtaining the total conductance of the Cu (111)/graphene/Cu (111) unit area under different stress strains by a nonequilibrium green's function method based on a density functional theory, and finally obtaining a relation curve of the strain and the Cu (111)/graphene/Cu (111) interface conductance value. The following trends can be clearly found from the simulation results: when the interface is stretched along the z direction, the total conductance of the system per unit area is gradually reduced; when the interface is stretched along the z direction, the total conductance per unit area of the system gradually decreases and increases, and referring to a strain-conductance graph of fig. 4, when the graphene/Cu (111) interface is subjected to a compressive stress (when the strain is less than 0), the conductivity of the interface is enhanced.
(6) According to a strain-conductance curve graph, the conductivity of the graphene/metal composite material interface is regulated and controlled by applying different stresses.
By utilizing the method, the conductivity of the graphene/metal interface can be efficiently and quickly improved by applying proper strain, and the method has important theoretical and practical significance for application design of the composite material in the aspect of electricity.
The steps can be repeated for different metal elements to obtain different strain-conductance value graphs. The conductivity of the graphene/metal composite material interface can be theoretically regulated and controlled by applying stress through a strain-conductivity curve, and the method can be used for simply and quickly evaluating the influence of stress strain on the conductivity of the graphene/metal interface so as to reduce the complexity and cost of experimental operation and reduce the cost of experiments, and has important theoretical and practical values.
Claims (6)
1. A design method for changing the conductivity of a graphene and metal interface through stress comprises the following steps:
(1) calculating the lattice parameters of the graphene and the base metal: obtaining lattice constants of graphene and base metal by a quantum mechanical first principle method in computational materials science;
(2) constructing a metal/graphene/metal composite interface model: the matrix metal is used as a main body, a metal/graphene/metal interface model is constructed by utilizing the lattice parameter of the metal, and the method adoptsThe graphene expansion surface;
(3) determining the morphology of the stably bonded metal/graphene/metal interface: determining the appearance of a stably combined metal/graphene/metal interface by calculating the interface combination energy of the graphene and the matrix metal;
(4) and (3) modeling and calculating theoretical conductance values of the interface model: performing device modeling on the stably combined composite interface by an unbalanced Green function method based on a density functional theory and simulating and calculating a conductance value of the interface;
(5) calculating and simulating the conductance value of the metal/graphene/metal interface model under different tension and compression conditions to obtain a relation curve graph of stress strain and the conductivity of the composite interface;
(6) and regulating and controlling the conductivity of the graphene/metal composite material interface by applying different stresses according to a strain-conductivity curve graph.
2. The design method for changing the conductivity of the interface between graphene and metal through stress according to claim 1, wherein: the base metal is copper, aluminum or magnesium; and repeating the steps aiming at different metal elements to obtain a strain-conductance curve graph.
3. The design method for changing the conductivity of the interface between graphene and metal through stress according to claim 1, wherein: when a metal/graphene/metal composite interface model is constructed, the thickness of the base metal layer is at least 12 atoms.
4. The design method for changing the conductivity of the interface between graphene and metal through stress according to claim 3, wherein: the base metal surface orientation is determined by simulation or experimental results.
5. The design method for changing the conductivity of the interface between graphene and metal through stress according to claim 1, wherein: the appearance of a stably combined metal/graphene/metal interface is preferentially determined through relative slip operation, and then the conductance value of the interface is calculated through an unbalanced Green function method based on a density functional theory.
6. The design method for changing the conductivity of the interface between graphene and metal through stress according to claim 5, wherein: determining the stably combined metal/graphene/metal interface morphology by taking the influence of the stably combined metal/graphene/metal interface morphology on a high interface binding energy value as a judgment basis, constructing a model aiming at different interface morphologies, calculating the interface binding energy, and screening the stably combined metal/graphene/metal interface morphology.
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CN107967403A (en) * | 2017-12-28 | 2018-04-27 | 南京理工大学 | The Forecasting Methodology of graphene/epoxy resin composite heat interfacial material thermal conductivity |
WO2020047500A1 (en) * | 2018-08-30 | 2020-03-05 | The Research Foundation For The State University Of New York | Graphene material-metal nanocomposites and processes of making and using same |
CN113322390A (en) * | 2021-06-04 | 2021-08-31 | 西北有色金属研究院 | Method for improving strength and conductivity matching of copper-based composite material based on in-situ reaction |
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CN107967403A (en) * | 2017-12-28 | 2018-04-27 | 南京理工大学 | The Forecasting Methodology of graphene/epoxy resin composite heat interfacial material thermal conductivity |
WO2020047500A1 (en) * | 2018-08-30 | 2020-03-05 | The Research Foundation For The State University Of New York | Graphene material-metal nanocomposites and processes of making and using same |
CN113322390A (en) * | 2021-06-04 | 2021-08-31 | 西北有色金属研究院 | Method for improving strength and conductivity matching of copper-based composite material based on in-situ reaction |
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JIAN WANG,ET AL.: "Effect of the graphene content on the microstructures and properties of graphene/aluminum composites", 《NEW CARBON MATERIALS》, vol. 34, no. 3, 31 December 2019 (2019-12-31), pages 275 - 285, XP085734905, DOI: 10.1016/S1872-5805(19)60016-8 * |
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