CN114994132A - Method for testing regulation and control of Rh-N4-graphene hydrogen evolution performance by stress - Google Patents
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Abstract
The invention discloses a method for testing the regulation and control of Rh-N4-graphene hydrogen evolution performance by stress, which comprises the following steps: s1, obtaining a stress range enabling Rh-N4-graphene to be in a stable state; s2, applying different stresses in a stress range to Rh-N4-graphene to obtain the electronic properties of the Rh-N4-graphene system under different stresses; s3, applying different stresses in a stress range to Rh-N4-graphene to obtain a 0-potential Rh-N4-graphene hydrogen evolution free energy diagram under different stresses; s4, constructing a stress-Rh-N4-graphene hydrogen evolution free energy curve diagram based on Rh-N4-graphene system electronic properties and combining with 0-potential Rh-N4-graphene hydrogen evolution free energy. The method can realize the purpose of discussing the activity of stress on the catalytic performance of the Rh-N4-graphene, and further realize the maximization of the atomic utilization rate when the Rh-N4-graphene is used as a hydrogen evolution reaction catalyst.
Description
Technical Field
The invention relates to the technical field of material performance research, in particular to a method for testing the regulation and control of Rh-N4-graphene hydrogen evolution performance by stress.
Background
The search and design of renewable clean energy sources has become one of the most important challenges in the world. Responding to this challenge is not only critical to global economy, but also helps mitigate the environmental and health hazards posed by fossil fuels. Hydrogen is the cleanest fuel and is considered one of the most promising energy sources for the twenty-first century. Hydrogen production by water electrolysis is a substitute for fossil fuel energy systems based on potential carbon dioxide emission.
Of all hydrogen evolution reaction catalysts, platinum (Pt) is by far the most effective catalyst, with a smaller overpotential in acidic solutions. However, the high cost and scarcity of platinum limits its use in the industrial production of hydrogen. Therefore, selecting an active, efficient, durable electrocatalyst from the earth's abundant resources remains a significant challenge for energy research. The monatomic catalyst can provide the most active centers and realize the maximum atom utilization efficiency, and has become a new research frontier in the field of catalysis in recent years, so that a new gate is opened for disclosing the catalytic process on an atomic scale. However, at present, the electrocatalysis mechanism research of the monatomic catalyst Rh-N4-graphene as the hydrogen evolution material is still not completely understood, so that the research on the stress is very important for the regulation and control of the hydrogen evolution electrocatalysis performance of the Rh-N4-graphene.
Disclosure of Invention
The invention aims to provide a method for testing the regulation and control of the stress on the hydrogen evolution performance of Rh-N4-graphene, so as to realize the discussion of the enthusiasm of the stress on the catalytic performance of Rh-N4-graphene, and further realize the maximization of the atom utilization rate when the Rh-N4-graphene is used as a hydrogen evolution reaction catalyst.
The invention is realized by the following technical scheme:
the method for testing the regulation and control of the Rh-N4-graphene hydrogen evolution performance by stress comprises the following steps:
s1, obtaining a stress range enabling Rh-N4-graphene to be in a stable state;
s2, applying different stresses in the stress range of S1 to Rh-N4-graphene to obtain the electronic properties of the Rh-N4-graphene system under different stresses;
s3, applying different stresses in the stress range of S1 to Rh-N4-graphene to obtain 0-potential Rh-N4-graphene hydrogen evolution free energy under different stresses;
s4, constructing a stress-Rh-N4-graphene hydrogen evolution free energy curve graph based on the Rh-N4-graphene system electronic performance obtained in the step S2 and the 0-potential Rh-N4-graphene hydrogen evolution free energy obtained in the step S3.
Step S1 of the method specifically includes applying different stresses to Rh-N4-graphene to obtain Rh-N4-graphene configurations under different stresses, and performing energy calculation and comparison on the Rh-N4-graphene configurations to determine stability. And then performing the operations of the step S2 and the step S3 in a stress range which can enable the Rh-N4-graphene to be in a stable state.
In the step S2, the electronic performance of the Rh-N4-graphene system can be judged according to the electron density near H atoms under different stresses: with the change in stress, if the electron density near the H atom decreases, i.e., the H atom loses more electrons, the loss of electrons from the H atom decreases the adsorption between H and the metal Rh, enhancing the desorption of the H atom, whereas with the change in stress, if the electron density near the H atom increases, i.e., the H atom loses less electrons, the loss of electrons from the H atom increases the adsorption between H and the metal Rh, weakening the desorption of the H atom.
The test proves that: with the increase of the stress applied to the Rh-N4-graphene, the electron density near the H atom is reduced, that is, the H atom loses more electrons, the loss of electrons of the H atom reduces the adsorption between the H and the metal Rh, and enhances the desorption of the H atom, so that with the increase of the stress, the adsorption between the H and the metal atom Rh is weakened, and the desorption of the H atom is enhanced.
In step S3 of the present invention, in order to further confirm that the adsorption between H and metal Rh is weakened with the increase of stress, a hydrogen evolution reaction path free energy diagram of Rh-N4-graphene at 0 potential under different stresses is established, hydrogen adsorption free energy under different pressures can be directly reflected by the hydrogen evolution reaction path free energy diagram at 0 potential, and with the increase of stress, the absolute value of the H adsorption free energy on the surface of Rh-N4-graphene is closer to 0, which means that the hydrogen evolution performance is better.
The test proves that: the free energy of H adsorption obtained under 10% stress is closer to 0, which shows that Rh-N4-graphene has the best hydrogen evolution performance under 10% stress.
The hydrogen evolution free energy can reflect the hydrogen evolution capacity of Rh-N4-graphene, so that the stress-Rh-N4-graphene hydrogen evolution free energy curve diagram constructed by the testing method can predict the hydrogen evolution capacity of Rh-N4-graphene in a scene without stress, so that a proper stress can be determined according to an actual application scene, and the atomic utilization rate is maximized when Rh-N4-graphene is used as a hydrogen evolution reaction catalyst, namely the hydrogen evolution capacity is maximized.
In conclusion, the testing method provided by the invention can discuss the positivity of stress on the catalytic performance of Rh-N4-graphene, and further maximize the atomic utilization rate when Rh-N4-graphene is used as a hydrogen evolution reaction catalyst.
Further, in step S1, the formation energy of Rh embedding into N4-graphene in Rh-N4-graphene under different stresses is calculated and recorded as E f By formation of energy E f And (6) judging the stability.
Furthermore, the energy of the Rh-N4-graphene system is formed by subtracting the energy of one metal atom in the Rh-N4-graphene system from the energy of the N4-graphene system.
Formation energy E f The specific calculation formula of (2) is as follows:
E f =E dopant+subs －E subs －E bulk
wherein, E dopant+subs Energy for Rh-N4-graphene System, E subs Energy of the N4-graphene system, E bulk Is the energy of one metal atom in the bulk Rh system.
Further, the specific steps of step S2 are as follows:
s21, establishing a differential charge density diagram corresponding to Rh-N4-graphene hydrogen evolution configuration under different stresses by changing the stress on the [100] crystal direction;
and S22, determining the electron gain and loss of the adsorbed atom H, and analyzing the electron performance.
Further, the specific steps of step S3 are as follows:
s31, establishing Rh-N4-graphene configurations under different stresses by changing the stress on the [100] crystal direction;
s32, obtaining system energy, surface energy and H after H adsorption in Rh-N4-graphene configuration under different stresses 2 Zero energy of molecular energy adsorption state H and gaseous H 2 Zero energy of (d);
s33, based on the step S32System energy, surface energy, one H after H adsorption 2 Zero energy of molecular energy adsorption state H and gaseous H 2 The zero energy of the energy is calculated to obtain the free energy G of hydrogen evolution of Rh atoms in Rh-N4-graphene under different stresses H ；
Free energy of hydrogen evolution G H The calculation formula of (c) is as follows:
∆G H =∆E H －T∆S H ＋∆E ZPE ；
∆E H =E(Subs+H)－E(Subs)＋E(H 2 )/2；
∆E ZPE =ZPE(H*)－1/2ZPE(H 2 )；
wherein, E H Represents the adsorption energy of H atoms on the surface, E (Subs + H) is the system energy after H adsorption, E (Subs) is the surface energy, E (H) 2 ) Is a H 2 The energy of the molecule; ZPE (H) is the zero energy of adsorption state H, ZPE (H) 2 ) Is in the gaseous state H 2 Zero energy, T Δ S H To let reaction entropy change, Δ S H =-1/2∆S H2 ，∆S H2 Is a gas H 2 Entropy under standard conditions, T is the reaction temperature.
S34, constructing a 0-potential Rh-N4-graphene hydrogen evolution free energy diagram under different stresses based on the hydrogen evolution free energy obtained in the step S33.
Further, the stress range of Rh-N4-graphene in a stable state is 0% -10%.
Compared with the prior art, the invention has the following advantages and beneficial effects:
1. on the basis of density functional theory calculation, the basic properties such as the electronic structure of Rh-N4-graphene are accurately understood, and the method is used for discussing the positivity of stress on the catalytic performance of Rh-N4-graphene.
2. When the testing method is used for Rh-N4-graphene serving as a hydrogen evolution reaction catalyst, the atom utilization rate can be maximized by applying a reasonable stress.
3. The invention provides a new idea for the performance research of the atomic catalyst including Rh-N4-graphene.
Drawings
The accompanying drawings, which are included to provide a further understanding of the embodiments of the invention and are incorporated in and constitute a part of this application, illustrate embodiment(s) of the invention and together with the description serve to explain the principles of the invention. In the drawings:
FIG. 1 is a flow chart of a test method provided in example 1;
FIG. 2 is a schematic diagram of Rh-N4-graphene configuration under no stress, wherein a is a top view and b is a side view;
FIG. 3 is a schematic configuration diagram of Rh-N4-graphene under different stresses;
FIG. 4 is a schematic diagram of the differential charge density of Rh-N4-graphene under different stresses;
FIG. 5 is a free energy diagram of hydrogen evolution reaction path of Rh-N4-graphene under 0% stress at 0 potential;
FIG. 6 is a free energy diagram of a hydrogen evolution reaction path of Rh-N4-graphene under 5% stress at 0 potential;
FIG. 7 is a free energy diagram of a hydrogen evolution reaction path of Rh-N4-graphene under 10% stress at 0 potential;
FIG. 8 is a graph of Rh-N4-graphene free energy as a function of stress.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is further described in detail below with reference to examples and accompanying drawings, and the exemplary embodiments and descriptions thereof are only used for explaining the present invention and are not meant to limit the present invention.
In general, the terms "comprises" and "comprising" merely indicate that steps and elements are included which are explicitly identified, that the steps and elements do not form an exclusive list, and that a method or apparatus may include other steps or elements. Flow charts are used in this description to illustrate operations performed by a system according to embodiments of the present description. It should be understood that the preceding or following operations are not necessarily performed in the exact order in which they are performed. Rather, the various steps may be processed in reverse order or simultaneously. Meanwhile, other operations may be added to the processes, or a certain step or several steps of operations may be removed from the processes.
Example 1:
as shown in fig. 1, the method for testing the regulation and control of Rh-N4-graphene hydrogen evolution energy by stress comprises the following steps:
s101, performing energy calculation and comparison on Rh-N4-graphene configurations under different stresses to determine stability;
in the embodiments of the present invention, please refer to fig. 2, in which fig. 2 shows the configuration of Rh-N4-graphene under no stress. Referring to FIG. 3, FIG. 3 is a graph showing a change [100]]Stress in the crystal direction, and establishing a Rh-N4-graphene configuration schematic diagram under different stresses; calculating the formation energy E of Rh embedded into N4-graphene in Rh-N4-graphene under different stresses f . Formation energy E f The specific calculation formula of (2) is as follows:
E f =E dopant+subs －E subs －E bulk
wherein E is dopant+subs Energy for Rh-N4-graphene System, E subs Energy of the N4-graphene system, E bulk Is the energy of one metal atom in the bulk Rh system.
0%, 5% and 10% (lattice constant at [100] with respect to the unstressed intrinsic Rh-N4-graphene]Percent compression of crystal orientation; energy of formation E under three stresses of 0% a = 14.80A, 5% a = 14.06A, and 10% a = 13.32A f -1.59eV, -1.82eV and-0.78 eV, respectively, and therefore Rh intercalation into N4-graphene at three stresses of 0%, 5% and 10% is stable, in particular: energy of Rh-N4-graphene system under different stresses: 0% (-647.20550 eV), 5% (-643.09187 eV), 10% (-637.14034 eV); the energy of the N4-graphene system is 0% (-638.36776 eV), 5% (-634.02297 eV), 10% (-629.11168 eV); the energy of one metal atom in the bulk Rh system is 0% (-7.2494443 eV), 5% (-7.2494443 eV), and 10% (-7.2494443 eV); the calculated formation energies E of 0%, 5% and 10% under three stresses f Respectively-1.59 eV, -1.82eV, and-0.78 eV.
S102, analyzing the change of the electronic property of the Rh-N4-graphene system under different stresses based on differential charge density;
in the embodiment of the invention, specifically, a differential charge density diagram corresponding to the Rh-N4-graphene hydrogen evolution configuration under different stresses is established by changing the stress in the [100] crystal direction, then the electron gain and loss of the adsorbed atom H is determined, and the electron performance is analyzed. Referring to fig. 4, fig. 4 is a schematic diagram of the differential charge density of Rh-N4-graphene under different stresses; as can be seen from the black area, as the [100] crystallographic stress increases, the electron density near the H atom decreases, i.e., the H atom loses more electrons, and the loss of electrons by the H atom reduces the adsorption between H and the metal Rh, enhancing the desorption of the H atom. Therefore, as the stress increases, the adsorption between H and the metal atom Rh is weakened, and the desorption of H atoms is enhanced.
S103, analyzing the electrocatalytic hydrogen production performance of Rh-N4-graphene based on Rh-N4-graphene with different stresses;
in the embodiment of the invention, in order to confirm that the adsorption between H and metal Rh is weakened along with the increase of stress, a hydrogen evolution reaction path free energy diagram of Rh-N4-graphene under 0 potential under different stresses is established. Specifically, the method comprises the following steps:
s1031, establishing Rh-N4-graphene configurations under different stresses by changing the stress on the [100] crystal direction;
s1032, obtaining system energy, surface energy and H after H adsorption in Rh-N4-graphene configuration under different stresses 2 Zero energy of molecular energy adsorption state H and gaseous H 2 Zero energy of (c);
s1033, system energy after H adsorption, surface energy, one H based on the H obtained in step S1032 2 Zero energy of molecular energy adsorption state H and gaseous H 2 The zero energy of the energy is calculated to obtain the free energy G of hydrogen evolution of Rh atoms in Rh-N4-graphene under different stresses H ；
Free energy of hydrogen evolution G H The calculation formula of (a) is as follows:
∆G H =∆E H －T∆S H ＋∆E ZPE ；
∆E H =E(Subs+H)－E(Subs)＋E(H 2 )/2；
∆E ZPE =ZPE(H*)－1/2ZPE(H 2 )；
wherein, E H Represents the adsorption energy of H atoms on the surface, E (Subs + H) is the system energy after H adsorption, E (Subs) is the surface energy，E(H 2 ) Is a H 2 The energy of the molecule; ZPE (H) is the zero energy of adsorption state H, ZPE (H) 2 ) Is in the gaseous state H 2 At zero point, T H To let reaction entropy change, Δ S H =-1/2∆S H2 ，∆S H2 Is a gas H 2 Entropy under standard conditions, T is the reaction temperature.
S1034, constructing a 0-potential Rh-N4-graphene hydrogen evolution free energy diagram under different stresses based on the hydrogen evolution free energy obtained in the step S1033.
Referring to fig. 5 to 7, fig. 5 is a free energy diagram of hydrogen evolution reaction path of Rh-N4-graphene under 0% stress at 0 potential; FIG. 6 is a free energy diagram of hydrogen evolution reaction path of Rh-N4-graphene under 5% stress at 0 potential; FIG. 7 is a free energy diagram of hydrogen evolution reaction path of Rh-N4-graphene under 10% stress at 0 potential. The hydrogen evolution free energy of the Rh-N4-graphene under the stress of 0 percent, 5 percent and 10 percent is-0.30 eV, -0.17eV and-0.07 eV respectively, and the absolute value of the H adsorption free energy of the surface of the Rh-N4-graphene is closer to 0 along with the increase of the stress, which means that the hydrogen evolution performance is better. Therefore, the free energy of H adsorption obtained under 10% stress is closer to 0, which shows that Rh-N4-graphene under 10% stress has the best hydrogen evolution performance.
Finally, based on the hydrogen evolution free energy curves of the Rh-N4-graphene under the stress of 0%, 5% and 10% shown in fig. 5 to 7 as-0.30 eV, -0.17eV and-0.07 eV, respectively, a stress-Rh-N4-graphene hydrogen evolution free energy curve graph is constructed, as shown in fig. 8, the stress-Rh-N4-graphene hydrogen evolution free energy curve graph shown in fig. 8 can be used to predict the hydrogen evolution capability of the Rh-N4-graphene under a non-stress scene, so as to determine an appropriate stress according to an actual application scene, so as to maximize the atomic utilization rate, i.e., the hydrogen evolution capability, when the Rh-N4-graphene is used as a hydrogen evolution reaction catalyst.
According to the test method, the stability is determined by calculating and comparing the energy of Rh-N4-graphene configurations under different stresses; analyzing the change of the electronic property of the Rh-N4-graphene system under different stresses based on differential charge density; the performance of Rh-N4-graphene electrocatalytic hydrogen production is analyzed based on Rh-N4-graphene with different stresses. The stability of Rh-N4-graphene is determined, and the internal reasons influencing the hydrogen evolution electrocatalysis performance of Rh-N4-graphene are analyzed; on the basis of density functional theory calculation, basic properties such as an electronic structure of Rh-N4-graphene are accurately understood, and the method is used for discussing the positivity of stress on the catalytic performance of Rh-N4-graphene.
The above-mentioned embodiments are intended to illustrate the objects, technical solutions and advantages of the present invention in further detail, and it should be understood that the above-mentioned embodiments are merely exemplary embodiments of the present invention, and are not intended to limit the scope of the present invention, and any modifications, equivalent substitutions, improvements and the like made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (6)
1. The method for testing the regulation and control of the Rh-N4-graphene hydrogen evolution performance by stress is characterized by comprising the following steps of:
s1, obtaining a stress range enabling Rh-N4-graphene to be in a stable state;
s2, applying different stresses in the stress range of S1 to Rh-N4-graphene to obtain the electronic properties of the Rh-N4-graphene system under different stresses;
s3, applying different stresses in the stress range of S1 to Rh-N4-graphene to obtain 0-potential Rh-N4-graphene hydrogen evolution free energy under different stresses;
s4, constructing a stress-Rh-N4-graphene hydrogen evolution free energy curve graph based on the Rh-N4-graphene system electronic performance obtained in the step S2 and the 0-potential Rh-N4-graphene hydrogen evolution free energy obtained in the step S3.
2. The method for testing the regulation and control of the hydrogen evolution performance of Rh-N4-graphene by stress according to claim 1, wherein in step S1, stability is judged by calculating the formation energy of Rh in Rh-N4-graphene embedded into N4-graphene under different stresses.
3. The method for testing the regulation and control of the hydrogen evolution performance of Rh-N4-graphene by stress according to claim 2, wherein the energy obtained by subtracting the energy of one metal atom in the Rh system from the difference between the energy of the Rh-N4-graphene system and the energy of the N4-graphene system is formed.
4. The method for testing the regulation and control of the hydrogen evolution performance of Rh-N4-graphene by stress according to claim 1, wherein the specific steps of step S2 are as follows:
s21, establishing a differential charge density diagram corresponding to the hydrogen evolution configuration of Rh-N4-graphene under different stresses by changing the stress on the [100] crystal direction;
and S22, determining the electron gain and loss of the adsorbed atom H, and analyzing the electron performance.
5. The method for testing the regulation and control of the hydrogen evolution performance of Rh-N4-graphene by stress according to claim 1, wherein the specific steps of step S3 are as follows:
s31, establishing Rh-N4-graphene configurations under different stresses by changing the stress on the [100] crystal direction;
s32, obtaining system energy, surface energy and H after H is adsorbed in Rh-N4-graphene configuration under different stresses 2 Zero energy of molecular energy adsorption state H and gaseous H 2 Zero energy of (d);
s33, based on the system energy after H adsorption, the surface energy and one H acquired in the step S32 2 Zero energy of molecular energy adsorption state H and gaseous H 2 Calculating to obtain the hydrogen evolution free energy of Rh-N4-graphene Rh atom pairs under different stresses;
s34, constructing a 0-potential Rh-N4-graphene hydrogen evolution free energy diagram under different stresses based on the hydrogen evolution free energy obtained in the step S33.
6. The method for testing the regulation and control of the hydrogen evolution performance of Rh-N4-graphene by stress according to claim 1, wherein the stress range for enabling Rh-N4-graphene to be in a stable state is 0% -10%.
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| CN114994132B (en) | 2022-11-01 |
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